Faïn, Xavier, Sophie Szopa, and Vaishali Naik, et al., January 2025: Preindustrial-to-present-day changes in atmospheric carbon monoxide: agreement and gaps between ice archives and global model reconstructions. Atmospheric Chemistry and Physics, 25(2), DOI:10.5194/acp-25-1105-20251105-1119. Abstract
Global chemistry–climate models (CCMs) play an important role in assessing the climate and air pollution implications of aerosols and chemically reactive gases. Evaluating these models under past conditions and constraining historical sources and sinks necessitate reliable records of atmospheric mixing ratios spanning preindustrial times. Such precious records were recently obtained for carbon monoxide (CO), documenting for the first time the evolution of this reactive compound over the industrial era. In this study, we compare the simulated atmospheric surface CO mixing ratios ([CO]) from two different sets of chemistry–climate models and emissions within the frameworks of CMIP5 and of CMIP6 (Coupled Model Intercomparison Project Phases 5 and 6) to recent bipolar ice archive reconstructions for the period spanning 1850 to the present. We analyse how historical (1850–2014) [CO] outputs from 16 ACCMIP (Atmospheric Chemistry and Climate Model Intercomparison Project) models and 7 AerChemMIP (Aerosol Chemistry Model Intercomparison Project) models over Greenland and Antarctica are able to capture both absolute values and trends recorded in multi-site ice archives. While most models underestimate [CO] at northern high latitudes, a reduction in this bias is observed between the ACCMIP and the AerChemMIP exercise. Over the 1980–2010 CE period (common era; all subsequent years in the paper are reported in CE), trends in ice archive and firn air observations and AerChemMIP outputs align remarkably well at northern and southern high latitudes, indicating improved quantification of anthropogenic CO emissions and the main CO sink (OH oxidation) compared to ACCMIP. From 1850 to 1980, AerChemMIP models and observations consistently show increasing [CO] in both the Northern Hemisphere (NH) and Southern Hemisphere (SH), suggesting a robust understanding of the CO budget evolution. However, a divergence in the [CO] growth rate emerges in the NH between models and observations over the 1920–1980 period, attributed to uncertainties in CO emission factors (EFs), particularly EFs for the RCO (residential, commercial, and other) and transportation sectors, although we cannot totally rule out the possibility that the CO record based on the Greenland ice archives may be biased high by CO chemical production processes occurring in the ice prior to the measurements (i.e. in situ CO production). In the Southern Hemisphere, AerChemMIP models simulate an increase in atmospheric [CO] from 1850 to 1980 that closely reproduces the observations (22 ± 10 ppb and 13 ± 7 ppb, respectively). Such agreement supports CMIP6 biomass burning CO emission inventories, which do not reveal a peak in CO emissions in the late 19th century. Furthermore, both SH models and observations reveal an accelerated growth rate in [CO] during 1945–1980 relative to 1850–1945, likely linked to increased anthropogenic transportation emissions.
Akritidis, Dimitris, Sara Bacer, Prodromos Zanis, Aristeidis K Georgoulias, Sourangsu Chowdhury, Larry W Horowitz, Vaishali Naik, Fiona M O'Connor, James Keeble, Philippe Le Sager, Twan van Noije, Putian Zhou, Steven T Turnock, J Jason West, Jos Lelieveld, and Andrea Pozzer, February 2024: Strong increase in mortality attributable to ozone pollution under a climate change and demographic scenario. Environmental Research Letters, 19(2), DOI:10.1088/1748-9326/ad2162. Abstract
Long-term exposure to ambient ozone (O3) is associated with excess respiratory mortality. Pollution emissions, demographic, and climate changes are expected to drive future ozone-related mortality. Here, we assess global mortality attributable to ozone according to an Intergovernmental Panel on Climate Change (IPCC) Shared Socioeconomic Pathway (SSP) scenario applied in Coupled Model Intercomparison Project Phase 6 (CMIP6) models, projecting a temperature increase of about 3.6 °C by the end of the century. We estimated ozone-related mortality on a global scale up to 2090 following the Global Burden of Disease (GBD) 2019 approach, using bias-corrected simulations from three CMIP6 Earth System Models (ESMs) under the SSP3-7.0 emissions scenario. Based on the three ESMs simulations, global ozone-related mortality by 2090 will amount to 2.79 M [95% CI 0.97 M–5.23 M] to 3.12 M [95% CI 1.11 M–5.75 M] per year, approximately ninefold that of the 327 K [95% CI 103 K–652 K] deaths per year in 2000. Climate change alone may lead to an increase of ozone-related mortality in 2090 between 42 K [95% CI −37 K–122 K] and 217 K [95% CI 68 K–367 K] per year. Population growth and ageing are associated with an increase in global ozone-related mortality by a factor of 5.34, while the increase by ozone trends alone ranges between factors of 1.48 and 1.7. Ambient ozone pollution under the high-emissions SSP3-7.0 scenario is projected to become a significant human health risk factor. Yet, optimizing living conditions and healthcare standards worldwide to the optimal ones today (application of minimum baseline mortality rates) will help mitigate the adverse consequences associated with population growth and ageing, and ozone increases caused by pollution emissions and climate change.
Fiedler, Stephanie, Vaishali Naik, Fiona M O'Connor, Christopher J Smith, Paul T Griffiths, and Ryan J Kramer, et al., March 2024: Interactions between atmospheric composition and climate change – progress in understanding and future opportunities from AerChemMIP, PDRMIP, and RFMIP. Geoscientific Model Development, 17(6), DOI:10.5194/gmd-17-2387-20242387–2417. Abstract
The climate science community aims to improve our understanding of climate change due to anthropogenic influences on atmospheric composition and the Earth's surface. Yet not all climate interactions are fully understood, and uncertainty in climate model results persists, as assessed in the latest Intergovernmental Panel on Climate Change (IPCC) assessment report. We synthesize current challenges and emphasize opportunities for advancing our understanding of the interactions between atmospheric composition, air quality, and climate change, as well as for quantifying model diversity. Our perspective is based on expert views from three multi-model intercomparison projects (MIPs) – the Precipitation Driver Response MIP (PDRMIP), the Aerosol Chemistry MIP (AerChemMIP), and the Radiative Forcing MIP (RFMIP). While there are many shared interests and specializations across the MIPs, they have their own scientific foci and specific approaches. The partial overlap between the MIPs proved useful for advancing the understanding of the perturbation–response paradigm through multi-model ensembles of Earth system models of varying complexity. We discuss the challenges of gaining insights from Earth system models that face computational and process representation limits and provide guidance from our lessons learned. Promising ideas to overcome some long-standing challenges in the near future are kilometer-scale experiments to better simulate circulation-dependent processes where it is possible and machine learning approaches where they are needed, e.g., for faster and better subgrid-scale parameterizations and pattern recognition in big data. New model constraints can arise from augmented observational products that leverage multiple datasets with machine learning approaches. Future MIPs can develop smart experiment protocols that strive towards an optimal trade-off between the resolution, complexity, and number of simulations and their length and, thereby, help to advance the understanding of climate change and its impacts.
Forster, Piers M., Christopher J Smith, Tristram Walsh, William F Lamb, Robin Lamboll, Bradley Hall, Mathias Hauser, Aurélien Ribes, Debbie Rosen, Nathan P Gillett, Matthew D Palmer, Joeri Rogelj, Karina von Schuckmann, Blair Trewin, Myles Allen, Robbie Andrew, Richard A Betts, Alex Borger, Tim Boyer, Jiddu A Broersma, Carlo Buontempo, Samantha Burgess, Chiara Cagnazzo, Lijing Cheng, Pierre Friedlingstein, Andrew Gettelman, Johannes Gütschow, Masayoshi Ishii, Stuart Jenkins, Xin Lan, Colin Morice, Jens Mühle, Christopher Kadow, John Kennedy, Rachel Killick, Paul Krummel, Jan C Minx, Gunnar Myhre, and Vaishali Naik, et al., June 2024: Indicators of global climate change 2023: Annual update of key indicators of the state of the climate system and human influence. Earth System Science Data, 16(6), DOI:10.5194/essd-16-2625-20242625–2658. Abstract
Intergovernmental Panel on Climate Change (IPCC) assessments are the trusted source of scientific evidence for climate negotiations taking place under the United Nations Framework Convention on Climate Change (UNFCCC). Evidence-based decision-making needs to be informed by up-to-date and timely information on key indicators of the state of the climate system and of the human influence on the global climate system. However, successive IPCC reports are published at intervals of 5–10 years, creating potential for an information gap between report cycles.
We follow methods as close as possible to those used in the IPCC Sixth Assessment Report (AR6) Working Group One (WGI) report. We compile monitoring datasets to produce estimates for key climate indicators related to forcing of the climate system: emissions of greenhouse gases and short-lived climate forcers, greenhouse gas concentrations, radiative forcing, the Earth's energy imbalance, surface temperature changes, warming attributed to human activities, the remaining carbon budget, and estimates of global temperature extremes. The purpose of this effort, grounded in an open-data, open-science approach, is to make annually updated reliable global climate indicators available in the public domain (https://doi.org/10.5281/zenodo.11388387, Smith et al., 2024a). As they are traceable to IPCC report methods, they can be trusted by all parties involved in UNFCCC negotiations and help convey wider understanding of the latest knowledge of the climate system and its direction of travel.
The indicators show that, for the 2014–2023 decade average, observed warming was 1.19 [1.06 to 1.30] °C, of which 1.19 [1.0 to 1.4] °C was human-induced. For the single-year average, human-induced warming reached 1.31 [1.1 to 1.7] °C in 2023 relative to 1850–1900. The best estimate is below the 2023-observed warming record of 1.43 [1.32 to 1.53] °C, indicating a substantial contribution of internal variability in the 2023 record. Human-induced warming has been increasing at a rate that is unprecedented in the instrumental record, reaching 0.26 [0.2–0.4] °C per decade over 2014–2023. This high rate of warming is caused by a combination of net greenhouse gas emissions being at a persistent high of 53±5.4 Gt CO2e yr−1 over the last decade, as well as reductions in the strength of aerosol cooling. Despite this, there is evidence that the rate of increase in CO2 emissions over the last decade has slowed compared to the 2000s, and depending on societal choices, a continued series of these annual updates over the critical 2020s decade could track a change of direction for some of the indicators presented here.
Kalisoras, Alkiviadis, Aristeidis K Georgoulias, Dimitris Akritidis, Robert J Allen, Vaishali Naik, Chaincy Kuo, Sophie Szopa, Pierre Nabat, Dirk Olivié, Twan van Noije, Philippe Le Sager, David Neubauer, Naga Oshima, Jane P Mulcahy, Larry W Horowitz, and Prodromos Zanis, July 2024: Decomposing the effective radiative forcing of anthropogenic aerosols based on CMIP6 Earth system models. Atmospheric Chemistry and Physics, 24(13), DOI:10.5194/acp-24-7837-20247837–7872. Abstract
Anthropogenic aerosols play a major role in the Earth–atmosphere system by influencing the Earth's radiative budget and precipitation and consequently the climate. The perturbation induced by changes in anthropogenic aerosols on the Earth's energy balance is quantified in terms of the effective radiative forcing (ERF). In this work, the present-day shortwave (SW), longwave (LW), and total (i.e., SW plus LW) ERF of anthropogenic aerosols is quantified using two different sets of experiments with prescribed sea surface temperatures (SSTs) from Earth system models (ESMs) participating in the Coupled Model Intercomparison Project Phase 6 (CMIP6): (a) time-slice pre-industrial perturbation simulations with fixed SSTs (piClim) and (b) transient historical simulations with time-evolving SSTs (histSST) over the historical period (1850–2014). ERF is decomposed into three components for both piClim and histSST experiments: (a) ERFARI, representing aerosol–radiation interactions; (b) ERFACI, accounting for aerosol–cloud interactions (including the semi-direct effect); and (c) ERFALB, which is due to temperature, humidity, and surface albedo changes caused by anthropogenic aerosols. We present spatial patterns at the top-of-atmosphere (TOA) and global weighted field means along with inter-model variability (1 standard deviation) for all SW, LW, and total ERF components (ERFARI, ERFACI, and ERFALB) and for every experiment used in this study. Moreover, the inter-model agreement and the robustness of our results are assessed using a comprehensive method as utilized in the IPCC Sixth Assessment Report. Based on piClim experiments, the total present-day (2014) ERF from anthropogenic aerosol and precursor emissions is estimated to be −1.11 ± 0.26 W m−2, mostly due to the large contribution of ERFACI to the global mean and to the inter-model variability. Based on the histSST experiments for the present-day period (1995–2014), similar results are derived, with a global mean total aerosol ERF of −1.28 ± 0.37 W m−2 and dominating contributions from ERFACI. The spatial patterns for total ERF and its components are similar in both the piClim and histSST experiments. Furthermore, implementing a novel approach to determine geographically the driving factor of ERF, we show that ERFACI dominates over the largest part of the Earth and that ERFALB dominates mainly over the poles, while ERFARI dominates over certain reflective surfaces. Analysis of the inter-model variability in total aerosol ERF shows that SW ERFACI is the main source of uncertainty predominantly over land regions with significant changes in aerosol optical depth (AOD), with eastern Asia contributing mostly to the inter-model spread of both ERFARI and ERFACI. The global spatial patterns of total ERF and its components from individual aerosol species, such as sulfates, organic carbon (OC), and black carbon (BC), are also calculated based on piClim experiments. The total ERF caused by sulfates (piClim-SO2) is estimated at −1.11 ± 0.31 W m−2, and the OC ERF (piClim-OC) is −0.35 ± 0.21 W m−2, while the ERF due to BC (piClim-BC) is 0.19 ± 0.18 W m−2. For sulfates and OC perturbation experiments, ERFACI dominates over the globe, whereas for BC perturbation experiments ERFARI dominates over land in the Northern Hemisphere and especially in the Arctic. Generally, sulfates dominate ERF spatial patterns, exerting a strongly negative ERF especially over industrialized regions of the Northern Hemisphere (NH), such as North America, Europe, and eastern and southern Asia. Our analysis of the temporal evolution of ERF over the historical period (1850–2014) reveals that ERFACI clearly dominates over ERFARI and ERFALB for driving the total ERF temporal evolution. Moreover, since the mid-1980s, total ERF has become less negative over eastern North America and western and central Europe, while over eastern and southern Asia there is a steady increase in ERF magnitude towards more negative values until 2014.
We describe the baseline model configuration and simulation characteristics of the Geophysical Fluid Dynamics Laboratory (GFDL)'s Land Model version 4.1 (LM4.1), which builds on component and coupled model developments over 2013–2019 for the coupled carbon-chemistry-climate Earth System Model Version 4.1 (ESM4.1) simulation as part of the sixth phase of the Coupled Model Intercomparison Project. Analysis of ESM4.1/LM4.1 is focused on biophysical and biogeochemical processes and interactions with climate. Key features include advanced vegetation dynamics and multi-layer canopy energy and moisture exchanges, daily fire, land use representation, and dynamic atmospheric dust coupling. We compare LM4.1 performance in the GFDL Earth System Model (ESM) configuration ESM4.1 to the previous generation component LM3.0 in the ESM2G configuration. ESM4.1/LM4.1 provides significant improvement in the treatment of ecological processes from GFDL's previous generation models. However, ESM4.1/LM4.1 likely overestimates the influence of land use and land cover change on vegetation characteristics, particularly on pasturelands, as it overestimates the competitiveness of grasses versus trees in the tropics, and as a result, underestimates present-day biomass and carbon uptake in comparison to observations.
Zhang, Shipeng, Vaishali Naik, David J Paynter, Simone Tilmes, and Jasmin G John, December 2024: Assessing GFDL-ESM4.1 climate responses to a stratospheric aerosol injection strategy intended to avoid overshoot 2.0°C warming. Geophysical Research Letters, 51(23), DOI:10.1029/2024GL113532. Abstract
In this work, we apply the GFDL Earth System Model (GFDL-ESM4.1) to explore the climate responses to a stratospheric aerosol injection (SAI) scenario that aims to restrict global warming to 2.0°C above pre-industrial levels (1850–1900) under the CMIP6 overshoot scenario (SSP5-34-OS). Simulations of this SAI scenario with the CESM Whole Atmosphere Community Climate Model (CESM2-WACCM6) showed nearly unchanged interhemispheric and pole-to-Equator surface temperature gradients relative to present-day conditions around 2020, and reduced global impacts, such as heatwaves, sea ice melting, and shifting precipitation patterns (Tilmes et al., 2020, https://doi.org/10.5194/esd-11-579-2020). However, model structural uncertainties can lead to varying climate projections under the same forcing. Implementing identical stratospheric aerosol radiative properties in GFDL-ESM4.1, which has a much lower Effective Climate Sensitivity compared to CESM2-WACCM6, resulted in a decrease in global-mean surface temperature by more than 1.5°C and a corresponding reduction in precipitation responses. Two major reasons contribute to the different temperature response between the two models: first, GFDL-ESM4.1 has less warming in the SSP534-OS scenario; second, GFDL-ESM4.1 has shown more pronounced cooling in response to the same stratospheric AOD perturbation. Notably, the Southern Hemisphere experiences substantial cooling compared to the Northern Hemisphere, accompanied by a northward shift of the Intertropical Convergence Zone (ITCZ). Furthermore, our analysis reveals that spatially heterogeneous forcing within the SAI scenario results in diverse climate feedback parameters in the GFDL-ESM4.1 model, through varying surface warming/cooling patterns. This research highlights the importance of considering model structural uncertainties and forcing spatial patterns for a comprehensive evaluation of future scenarios and geoengineering strategies.
Ahsan, Hamza, Hailong Wang, Jingbo Wu, Mingxuan Wu, Steven J Smith, Susanne E Bauer, Harrison Suchyta, Dirk Olivié, Gunnar Myhre, Hitoshi Matsui, Huisheng Bian, Jean-Francois Lamarque, Kenneth S Carslaw, Larry W Horowitz, Leighton Regayre, Mian Chin, Michael Schulz, Ragnhild Bieltvedt-Skeie, Toshihiko Takemura, and Vaishali Naik, December 2023: The Emissions Model Intercomparison Project (Emissions-MIP): Quantifying model sensitivity to emission characteristics. Atmospheric Chemistry and Physics, 23(23), DOI:10.5194/acp-23-14779-202314779–14799. Abstract
Anthropogenic emissions of aerosols and precursor compounds are known to significantly affect the energy balance of the Earth–atmosphere system, alter the formation of clouds and precipitation, and have a substantial impact on human health and the environment. Global models are an essential tool for examining the impacts of these emissions. In this study, we examine the sensitivity of model results to the assumed height of SO2 injection, seasonality of SO2 and black carbon (BC) particulate emissions, and the assumed fraction of SO2 emissions that is injected into the atmosphere as particulate phase sulfate (SO4) in 11 climate and chemistry models, including both chemical transport models and the atmospheric component of Earth system models. We find large variation in atmospheric lifetime across models for SO2, SO4, and BC, with a particularly large relative variation for SO2, which indicates that fundamental aspects of atmospheric sulfur chemistry remain uncertain. Of the perturbations examined in this study, the assumed height of SO2 injection had the largest overall impacts, particularly on global mean net radiative flux (maximum difference of −0.35 W m−2), SO2 lifetime over Northern Hemisphere land (maximum difference of 0.8 d), surface SO2 concentration (up to 59 % decrease), and surface sulfate concentration (up to 23 % increase). Emitting SO2 at height consistently increased SO2 and SO4 column burdens and shortwave cooling, with varying magnitudes, but had inconsistent effects across models on the sign of the change in implied cloud forcing. The assumed SO4 emission fraction also had a significant impact on net radiative flux and surface sulfate concentration. Because these properties are not standardized across models this is a source of inter-model diversity typically neglected in model intercomparisons. These results imply a need to ensure that anthropogenic emission injection height and SO4 emission fraction are accurately and consistently represented in global models.
Chua, Glen, Vaishali Naik, and Larry W Horowitz, April 2023: Exploring the drivers of tropospheric hydroxyl radical trends in the Geophysical Fluid Dynamics Laboratory AM4.1 atmospheric chemistry–climate model. Atmospheric Chemistry and Physics, 23(8), DOI:10.5194/acp-23-4955-20234955-4975. Abstract
We explore the sensitivity of modeled tropospheric hydroxyl (OH) concentration trends to meteorology and near-term climate forcers (NTCFs), namely methane (CH4) nitrogen oxides (NOX = NO2 + NO) carbon monoxide (CO), non-methane volatile organic compounds (NMVOCs) and ozone-depleting substances (ODSs), using the Geophysical Fluid Dynamics Laboratory (GFDL)'s atmospheric chemistry–climate model, the Atmospheric Model version 4.1 (AM4.1), driven by emissions inventories developed for the Sixth Coupled Model Intercomparison Project (CMIP6) and forced by observed sea surface temperatures and sea ice prepared in support of the CMIP6 Atmospheric Model Intercomparison Project (AMIP) simulations. We find that the modeled tropospheric air-mass-weighted mean [OH] has increased by ∼5 % globally from 1980 to 2014. We find that NOx emissions and CH4 concentrations dominate the modeled global trend, while CO emissions and meteorology were also important in driving regional trends. Modeled tropospheric NO2 column trends are largely consistent with those retrieved from the Ozone Monitoring Instrument (OMI) satellite, but simulated CO column trends generally overestimate those retrieved from the Measurements of Pollution in The Troposphere (MOPITT) satellite, possibly reflecting biases in input anthropogenic emission inventories, especially over China and South Asia.
Forster, Piers M., Christopher J Smith, Tristram Walsh, William F Lamb, Robin Lamboll, Mathias Hauser, Aurélien Ribes, Debbie Rosen, Nathan P Gillett, Matthew D Palmer, Joeri Rogelj, Karina von Schuckmann, Sonia I Seneviratne, Blair Trewin, Xuebin Zhang, Myles Allen, Robbie Andrew, Arlene Birt, Alex Borger, Tim Boyer, Jiddu A Broersma, Lijing Cheng, Frank Dentener, Pierre Friedlingstein, José M Gutiérrez, Johannes Gütschow, Bradley Hall, Masayoshi Ishii, Stuart Jenkins, Xin Lan, June-Yi Lee, Colin Morice, Christopher Kadow, John Kennedy, Rachel Killick, Jan C Minx, and Vaishali Naik, et al., June 2023: Indicators of Global Climate Change 2022: annual update of large-scale indicators of the state of the climate system and human influence. Earth System Science Data, 15(6), DOI:10.5194/essd-15-2295-20232295-2327.
Stratospheric injections of sulfur dioxide from major volcanic eruptions perturb the Earth's global radiative balance and dominate variability in stratospheric sulfur loading. The atmospheric component of the GFDL Earth System Model (ESM4.1) uses a bulk aerosol scheme and previously prescribed the distribution of aerosol optical properties in the stratosphere. To quantify volcanic contributions to the stratospheric sulfur cycle and the resulting climate impact, we modified ESM4.1 to simulate stratospheric sulfate aerosols prognostically. Driven by explicit volcanic emissions of aerosol precursors and non-volcanic sources, we conduct ESM4.1 simulations from 1989 to 2014, with a focus on the Mt. Pinatubo eruption. We evaluate our interactive representation of the stratospheric sulfur cycle against data from Moderate Resolution Imaging Spectroradiometer, Multi-angle Imaging SpectroRadiometer, Advanced Very High Resolution Radiometer, High Resolution Infrared Radiation Sounder, and Stratospheric Aerosol and Gas Experiment II. To assess the key processes associated with volcanic aerosols, we performed a sensitivity analysis of sulfate burden from the Mt. Pinatubo eruption by varying injection heights, emission amount, and stratospheric sulfate's dry effective radius. We find that the simulated stratospheric sulfate mass burden and aerosol optical depth in the model are sensitive to these parameters, especially volcanic SO2 injection height, and the optimal combination of parameters depends on the metric we evaluate.
Kalisoras, Alkiviadis, Aristeidis K Georgoulias, Dimitris Akritidis, Robert J Allen, Vaishali Naik, and Prodromos Zanis, August 2023: Estimating the effective radiative forcing of anthropogenic aerosols with the use of CMIP6 Earth System Models. Environmental Sciences Proceedings, 26(1), DOI:10.3390/environsciproc2023026040. Abstract
We investigate the effective radiative forcing (ERF) of anthropogenic aerosols using simulations from seven Earth System Models participating in the Coupled Model Intercomparison Project Phase 6 (CMIP6). The ERF of individual aerosol species (black carbon, organic carbon, sulphates) is quantified along with the all-aerosol ERF and decomposed into its aerosol–radiation interactions (ARI), aerosol–cloud interactions (ACI) and surface albedo (ALB) components, using the method proposed by Ghan in 2013. We find that the total anthropogenic aerosol ERF at the top of the atmosphere (TOA) is negative, mainly due to aerosol–cloud interactions. Sulphates exhibit a strongly negative ERF especially over industrialized regions of the Northern Hemisphere, such as Europe, North America, East and South Asia, while black carbon exerts a positive ERF predominantly over East and South Asia.
Biogenic secondary organic aerosols (SOAs) contribute to a large fraction of fine aerosols globally, impacting air quality and climate. The formation of biogenic SOA depends on not only emissions of biogenic volatile organic compounds (BVOCs) but also anthropogenic pollutants including primary organic aerosol, sulfur dioxide (SO2), and nitrogen oxides (NOx). However, the anthropogenic impact on biogenic SOA production (AIBS) remains unclear. Here we use the decadal trend and variability in observed organic aerosol (OA) in the southeast US, combined with a global chemistry–climate model, to better constrain AIBS. We show that the reduction in SO2 emissions can only explain 40 % of the decreasing decadal trend of OA in this region, constrained by the low summertime month-to-month variability in surface OA. We hypothesize that the rest of the OA decreasing trend is largely due to a reduction in NOx emissions. By implementing a scheme for monoterpene SOA with enhanced sensitivity to NOx, our model can reproduce the decadal trend and variability in OA in this region. Extending to a centennial scale, our model shows that global SOA production increases by 36 % despite BVOC reductions from the preindustrial period to the present day, largely amplified by AIBS. Our work suggests a strong coupling between anthropogenic and biogenic emissions in biogenic SOA production that is missing from current climate models.
The Mediterranean is a projected hot spot for climate change, with significant warming and rainfall reductions. We use climate model ensembles to explore whether these Mediterranean rainfall declines could be reversed in response to greenhouse gas reductions. While the summer Mediterranean rainfall decline is reversed, winter rainfall continues to decline. The continued decline results from prolonged weakening of Atlantic Ocean poleward heat transport that combines with greenhouse gas reductions to cool the subpolar North Atlantic, inducing atmospheric circulation changes that favor continued Mediterranean drying. This is a potential “surprise” in the climate system, whereby changes in one component (Atlantic Ocean circulation) alter how another component (Mediterranean rainfall) responds to greenhouse gas reductions. Such surprises could complicate climate change mitigation efforts.
We analyze the relationship between fine particulate matter (PM2.5) and meteorology in winter in the Indo-Gangetic Plain (IGP). We find that the concentration of PM2.5 exhibits similar increase with decreasing surface wind speed in 15 out of 18 cities considered. Using this observed relationship, we estimate that the reduction of surface wind speed with increasing CO2 simulated by models participating in the Coupled Model Intercomparison Project Phase 6 will result in higher average wintertime PM2.5 concentrations (1% per degree K of global warming) and more frequent high-pollution events. This observation-based estimate is qualitatively consistent with the simulated response of black carbon to global warming inferred from the AerChemMIP ssp370SST and ssp370pdSST experiments. We hypothesize that a reduction in the frequency and intensity of western disturbances with increasing CO2 may contribute to the reduction in the surface wind in the IGP.
Quaas, Johannes, Hailing Jia, C A Smith, Anna Lea Albright, Wenche Aas, Nicolas Bellouin, Olivier Boucher, Marie Doutriaux-Boucher, Piers M Forster, Daniel Grosvenor, Stuart Jenkins, Zbigniew Klimont, Norman G Loeb, Xiaoyan Ma, Vaishali Naik, Fabien Paulot, Philip Stier, M Wild, Gunnar Myhre, and M Schulz, September 2022: Robust evidence for reversal of the trend in aerosol effective climate forcing. Atmospheric Chemistry and Physics, 22(18), DOI:10.5194/acp-22-12221-202212221-12239. Abstract
Anthropogenic aerosols exert a cooling influence that offsets part of the greenhouse gas warming. Due to their short tropospheric lifetime of only several days, the aerosol forcing responds quickly to emissions. Here, we present and discuss the evolution of the aerosol forcing since 2000. There are multiple lines of evidence that allow us to robustly conclude that the anthropogenic aerosol effective radiative forcing (ERF) – both aerosol–radiation interactions (ERFari) and aerosol–cloud interactions (ERFaci) – has become less negative globally, i.e. the trend in aerosol effective radiative forcing changed sign from negative to positive. Bottom-up inventories show that anthropogenic primary aerosol and aerosol precursor emissions declined in most regions of the world; observations related to aerosol burden show declining trends, in particular of the fine-mode particles that make up most of the anthropogenic aerosols; satellite retrievals of cloud droplet numbers show trends in regions with aerosol declines that are consistent with these in sign, as do observations of top-of-atmosphere radiation. Climate model results, including a revised set that is constrained by observations of the ocean heat content evolution show a consistent sign and magnitude for a positive forcing relative to the year 2000 due to reduced aerosol effects. This reduction leads to an acceleration of the forcing of climate change, i.e. an increase in forcing by 0.1 to 0.3 W m−2, up to 12 % of the total climate forcing in 2019 compared to 1750 according to the Intergovernmental Panel on Climate Change (IPCC).
Zanis, Prodromos, Dimitris Akritidis, Steven T Turnock, Vaishali Naik, Sophie Szopa, Aristeidis K Georgoulias, Susanne E Bauer, Makoto Deushi, and Larry W Horowitz, et al., January 2022: Climate change penalty and benefit on surface ozone: A global perspective based on CMIP6 earth system models. Environmental Research Letters, 17(2), DOI:10.1088/1748-9326/ac4a34. Abstract
This work presents an analysis of the effect of climate change on surface ozone discussing the related penalties and benefits around the globe from the global modelling perspective based on simulations with five CMIP6 (Coupled Model Intercomparison Project Phase 6) Earth System Models. As part of AerChemMIP (Aerosol Chemistry Model Intercomparison Project) all models conducted simulation experiments considering future climate (ssp370SST) and present-day climate (ssp370pdSST) under the same future emissions trajectory (SSP3-7.0). A multi-model global average climate change benefit on surface ozone of −0.96 ± 0.07 ppbv °C−1 is calculated which is mainly linked to the dominating role of enhanced ozone destruction with higher water vapour abundances under a warmer climate. Over regions remote from pollution sources, there is a robust decline in mean surface ozone concentration on an annual basis as well as for boreal winter and summer varying spatially from −0.2 to −2 ppbv °C−1, with strongest decline over tropical oceanic regions. The implication is that over regions remote from pollution sources (except over the Arctic) there is a consistent climate change benefit for baseline ozone due to global warming. However, ozone increases over regions close to anthropogenic pollution sources or close to enhanced natural biogenic volatile organic compounds emission sources with a rate ranging regionally from 0.2 to 2 ppbv C−1, implying a regional surface ozone penalty due to global warming. Overall, the future climate change enhances the efficiency of precursor emissions to generate surface ozone in polluted regions and thus the magnitude of this effect depends on the regional emission changes considered in this study within the SSP3_7.0 scenario. The comparison of the climate change impact effect on surface ozone versus the combined effect of climate and emission changes indicates the dominant role of precursor emission changes in projecting surface ozone concentrations under future climate change scenarios.
Zeng, Guang, Olaf Morgenstern, Jonny Williams, Fiona M O'Connor, Paul T Griffiths, James Keeble, Makoto Deushi, Larry W Horowitz, Vaishali Naik, Louisa K Emmons, N Luke Abraham, Alexander T Archibald, Susanne E Bauer, Birgit Hassler, Martine Michou, Michael J Mills, Lee T Murray, Naga Oshima, Lori T Sentman, Simone Tilmes, Kostas Tsigaridis, and Paul J Young, August 2022: Attribution of stratospheric and tropospheric ozone changes between 1850 and 2014 in CMIP6 models. JGR Atmospheres, 127(16), DOI:10.1029/2022JD036452. Abstract
We quantify the impacts of halogenated ozone-depleting substances (ODSs), greenhouse gases (GHGs), and short-lived ozone precursors on ozone changes between 1850 and 2014 using single-forcing perturbation simulations from several Earth system models with interactive chemistry participating in the Coupled Model Intercomparison Project Aerosol and Chemistry Model Intercomparison Project. We present the responses of ozone to individual forcings and an attribution of changes in ozone columns and vertically resolved stratospheric and tropospheric ozone to these forcings. We find that whilst substantial ODS-induced ozone loss dominates the stratospheric ozone changes since the 1970s, in agreement with previous studies, increases in tropospheric ozone due to increases in short-lived ozone precursors and methane since the 1950s make increasingly important contributions to total column ozone (TCO) changes. Increases in methane also lead to substantial extra-tropical stratospheric ozone increases. Impacts of nitrous oxide and carbon dioxide on stratospheric ozone are significant but their impacts on TCO are small overall due to several opposing factors and are also associated with large dynamical variability. The multi-model mean (MMM) results show a clear change in the stratospheric ozone trends after 2000 due to now declining ODSs, but the trends are generally not significantly positive, except in the extra-tropical upper stratosphere, due to relatively small changes in forcing over this period combined with large model uncertainty. Although the MMM ozone compares well with the observations, the inter-model differences are large primarily due to the large differences in the models' representation of ODS-induced ozone depletion.
Allen, Robert J., Larry W Horowitz, Vaishali Naik, Naga Oshima, Fiona M O'Connor, Steven T Turnock, Sungbo Shim, Philippe Le Sager, Twan van Noije, Kostas Tsigaridis, Susanne E Bauer, Lori T Sentman, and Jasmin G John, et al., February 2021: Significant climate benefits from near-term climate forcer mitigation in spite of aerosol reductions. Environmental Research Letters, 16(3), DOI:10.1088/1748-9326/abe06b. Abstract
Near-term climate forcers (NTCFs), including aerosols and chemically reactive gases such as tropospheric ozone and methane, offer a potential way to mitigate climate change and improve air quality—so called 'win-win' mitigation policies. Prior studies support improved air quality under NTCF mitigation, but with conflicting climate impacts that range from a significant reduction in the rate of global warming to only a modest impact. Here, we use state-of-the-art chemistry-climate model simulations conducted as part of the Aerosol and Chemistry Model Intercomparison Project (AerChemMIP) to quantify the 21st-century impact of NTCF reductions, using a realistic future emission scenario with a consistent air quality policy. Non-methane NTCF (NMNTCF; aerosols and ozone precursors) mitigation improves air quality, but leads to significant increases in global mean precipitation of 1.3% by mid-century and 1.4% by end-of-the-century, and corresponding surface warming of 0.23 and 0.21 K. NTCF (all-NTCF; including methane) mitigation further improves air quality, with larger reductions of up to 45% for ozone pollution, while offsetting half of the wetting by mid-century (0.7% increase) and all the wetting by end-of-the-century (non-significant 0.1% increase) and leading to surface cooling of −0.15 K by mid-century and −0.50 K by end-of-the-century. This suggests that methane mitigation offsets warming induced from reductions in NMNTCFs, while also leading to net improvements in air quality.
Arias, Paola A., Nicolas Bellouin, Erika Coppola, Richard G Jones, Gerhard Krinner, Jochem Marotzke, and Vaishali Naik, et al., in press: Technical Summary. In Climate Change 2021: The Physical Science Basis. Contribution of Working Group I to the Sixth Assessment Report of the Intergovernmental Panel on Climate Change, , Cambridge University Press. August 2021.
Canadell, Josep G., Pedro M S Monteiro, Marcos H Costa, Leticia Cotrim da Cunha, Peter Cox, Alexey V Eliseev, Stephanie A Henson, Masao Ishii, Samuel Jaccard, Charles D Koven, Annalea Lohila, Prabir K Patra, Shilong Piao, Joeri Rogelj, Stephen Syampungani, Sönke Zaehle, Kirsten Zickfield, Jian He, and Vaishali Naik, et al., in press: Global Carbon and other Biogeochemical Cycles and Feedbacks. In Climate Change 2021: The Physical Science Basis. Contribution of Working Group I to the Sixth Assessment Report of the Intergovernmental Panel on Climate Change, , Cambridge University Press. August 2021.
Griffiths, Paul T., Lee T Murray, Guang Zeng, Youngsub Matthew Shin, N Luke Abraham, Alexander T Archibald, Makoto Deushi, Louisa K Emmons, Ian E Galbally, Birgit Hassler, Larry W Horowitz, James Keeble, Jane Liu, O Moeini, and Vaishali Naik, et al., March 2021: Tropospheric ozone in CMIP6 Simulations. Atmospheric Chemistry and Physics, 21(5), DOI:10.5194/acp-21-4187-20214187-4218. Abstract
The evolution of tropospheric ozone from 1850 to 2100 has been studied using data from Phase 6 of the Coupled Model Intercomparison Project (CMIP6). We evaluate long-term changes using coupled atmosphere–ocean chemistry–climate models, focusing on the CMIP Historical and ScenarioMIP ssp370 experiments, for which detailed tropospheric-ozone diagnostics were archived. The model ensemble has been evaluated against a suite of surface, sonde and satellite observations of the past several decades and found to reproduce well the salient spatial, seasonal and decadal variability and trends. The multi-model mean tropospheric-ozone burden increases from 247 ± 36 Tg in 1850 to a mean value of 356 ± 31 Tg for the period 2005–2014, an increase of 44 %. Modelled present-day values agree well with previous determinations (ACCENT: 336 ± 27 Tg; Atmospheric Chemistry and Climate Model Intercomparison Project, ACCMIP: 337 ± 23 Tg; Tropospheric Ozone Assessment Report, TOAR: 340 ± 34 Tg). In the ssp370 experiments, the ozone burden increases to 416 ± 35 Tg by 2100. The ozone budget has been examined over the same period using lumped ozone production (PO3) and loss (LO3) diagnostics. Both ozone production and chemical loss terms increase steadily over the period 1850 to 2100, with net chemical production (PO3-LO3) reaching a maximum around the year 2000. The residual term, which contains contributions from stratosphere–troposphere transport reaches a minimum around the same time before recovering in the 21st century, while dry deposition increases steadily over the period 1850–2100. Differences between the model residual terms are explained in terms of variation in tropopause height and stratospheric ozone burden.
The hydroxyl radical (OH) is extremely reactive in the atmosphere and able to destroy many other chemicals, such as methane, a strong greenhouse gas that contributes significantly to global warming. Therefore, OH is very important for methane concentrations and lifetime. Changes in the meteorological features (e.g., temperature, wind patterns, and relative humidity) would affect OH in the atmosphere. In this study, we use a three-dimensional numerical model to understand the meteorological impacts on OH and the resulting impacts on methane budget and lifetime over 1980–2017. With different meteorological datasets, we find there is a 2% difference in global mean tropospheric OH concentrations, with much larger differences over tropics. We calculate methane sources and loss due to OH and find an 11.2 Tg yr−1 difference in the global mean methane sources with 8 Tg yr−1 difference in the tropics, and 0.24 years difference in methane lifetime between the two meteorological datasets.
The Coronavirus Disease 2019 (COVID‐19) pandemic led to a widespread reduction in aerosol emissions. Using satellite observations and climate model simulations, we study the underlying mechanisms of the large decreases in solar clear‐sky reflection (3.8 W m−2 or 7%) and aerosol optical depth (0.16 W m−2 or 32%) observed over the East Asian Marginal Seas in March 2020. By separating the impacts from meteorology and emissions in the model simulations, we find that about one‐third of the clear‐sky anomalies can be attributed to pandemic‐related emission reductions, and the rest to weather variability and long‐term emission trends. The model is skillful at reproducing the observed interannual variations in solar all‐sky reflection, but no COVID‐19 signal is discerned. The current observational and modeling capabilities will be critical for monitoring, understanding, and predicting the radiative forcing and climate impacts of the ongoing crisis.
The hydroxyl radical (OH) sets the oxidative capacity of the atmosphere and, thus, profoundly affects the removal rate of pollutants and reactive greenhouse gases. While observationally derived constraints exist for global annual mean present-day OH abundances and interannual variability, OH estimates for past and future periods rely primarily on global atmospheric chemistry models. These models disagree ± 30% in mean OH and in its changes from the preindustrial to late 21st century, even when forced with identical anthropogenic emissions. A simple steady-state relationship that accounts for ozone photolysis frequencies, water vapor, and the ratio of reactive nitrogen to carbon emissions explains temporal variability within most models, but not intermodel differences. Here, we show that departure from the expected relationship reflects the treatment of reactive oxidized nitrogen species (NOy) and the fraction of emitted carbon that reacts within each chemical mechanism, which remain poorly known due to a lack of observational data. Our findings imply a need for additional observational constraints on NOy partitioning and lifetime, especially in the remote free troposphere, as well as the fate of carbon-containing reaction intermediates to test models, thereby reducing uncertainties in projections of OH and, hence, lifetimes of pollutants and greenhouse gases.
Hydrogen (H2) has been proposed as an alternative energy carrier to reduce the carbon footprint and associated radiative forcing of the current energy system. Here, we describe the representation of H2 in the GFDL-AM4.1 model including updated emission inventories and improved representation of H2 soil removal, the dominant sink of H2. The model best captures the overall distribution of surface H2, including regional contrasts between climate zones, when vd(H2) is modulated by soil moisture, temperature, and soil carbon content. We estimate that the soil removal of H2 increases with warming (2–4% per K), with large uncertainties stemming from different regional response of soil moisture and soil carbon. We estimate that H2 causes an indirect radiative forcing of 0.84 mW m−2/(Tg(H2)yr−1) or 0.13 mW m−2 ppbv−1, primarily due to increasing CH4 lifetime and stratospheric water vapor production.
Szopa, Sophie, Vaishali Naik, Bhupesh Adhikary, Paulo Artaxo, Terje Berntsen, William D Collins, Sandro Fuzzi, Laura Gallardo, Astrid Kiendler-Scharr, Zbigniew Klimont, Hong Liao, Nadine Unger, Prodromos Zanis, Paul Ginoux, Jian He, and Fabien Paulot, et al., August 2021: Short-Lived Climate Forcers In Climate Change 2021: The Physical Science Basis. Contribution of Working Group I to the Sixth Assessment Report of the Intergovernmental Panel on Climate Change, Cambridge, United Kingdom and New York, NY, USA, Cambridge University Press, DOI:10.1017/9781009157896.008817-922.
Thornhill, Gillian D., William J Collins, Ryan J Kramer, Dirk Olivié, Ragnhild B Skeie, Fiona M O'Connor, N Luke Abraham, Ramiro Checa-Garcia, Susanne E Bauer, Makoto Deushi, Louisa K Emmons, Piers M Forster, Larry W Horowitz, Ben Johnson, James Keeble, Jean-Francois Lamarque, Martine Michou, Michael J Mills, Jane P Mulcahy, Gunnar Myhre, Pierre Nabat, and Vaishali Naik, et al., January 2021: Effective radiative forcing from emissions of reactive gases and aerosols – a multi-model comparison. Atmospheric Chemistry and Physics, 21(2), DOI:10.5194/acp-21-853-2021853-874. Abstract
This paper quantifies the pre-industrial (1850) to present-day (2014) effective radiative forcing (ERF) of anthropogenic emissions of NOX, volatile organic compounds (VOCs; including CO), SO2, NH3, black carbon, organic carbon, and concentrations of methane, N2O and ozone-depleting halocarbons, using CMIP6 models. Concentration and emission changes of reactive species can cause multiple changes in the composition of radiatively active species: tropospheric ozone, stratospheric ozone, stratospheric water vapour, secondary inorganic and organic aerosol, and methane. Where possible we break down the ERFs from each emitted species into the contributions from the composition changes. The ERFs are calculated for each of the models that participated in the AerChemMIP experiments as part of the CMIP6 project, where the relevant model output was available.
The 1850 to 2014 multi-model mean ERFs (± standard deviations) are −1.03 ± 0.37 W m−2 for SO2 emissions, −0.25 ± 0.09 W m−2 for organic carbon (OC), 0.15 ± 0.17 W m−2 for black carbon (BC) and −0.07 ± 0.01 W m−2 for NH3. For the combined aerosols (in the piClim-aer experiment) it is −1.01 ± 0.25 W m−2. The multi-model means for the reactive well-mixed greenhouse gases (including any effects on ozone and aerosol chemistry) are 0.67 ± 0.17 W m−2 for methane (CH4), 0.26 ± 0.07 W m−2 for nitrous oxide (N2O) and 0.12 ± 0.2 W m−2 for ozone-depleting halocarbons (HC). Emissions of the ozone precursors nitrogen oxides (NOx), volatile organic compounds and both together (O3) lead to ERFs of 0.14 ± 0.13, 0.09 ± 0.14 and 0.20 ± 0.07 W m−2 respectively. The differences in ERFs calculated for the different models reflect differences in the complexity of their aerosol and chemistry schemes, especially in the case of methane where tropospheric chemistry captures increased forcing from ozone production.
Thornhill, Gillian D., William J Collins, Dirk Olivié, Ragnhild B Skeie, Alexander T Archibald, Susanne E Bauer, Ramiro Checa-Garcia, Stephanie Fiedler, Gerd Folberth, Ada Gjermundsen, Larry W Horowitz, Jean-Francois Lamarque, Martine Michou, Jane P Mulcahy, Pierre Nabat, Vaishali Naik, Fiona M O'Connor, and Fabien Paulot, et al., January 2021: Climate-driven chemistry and aerosol feedbacks in CMIP6 Earth system models. Atmospheric Chemistry and Physics, 21(2), DOI:10.5194/acp-21-1105-20211105-1126. Abstract
Feedbacks play a fundamental role in determining the magnitude of the response of the climate system to external forcing, such as from anthropogenic emissions. The latest generation of Earth system models includes aerosol and chemistry components that interact with each other and with the biosphere. These interactions introduce a complex web of feedbacks that is important to understand and quantify.
This paper addresses multiple pathways for aerosol and chemical feedbacks in Earth system models. These focus on changes in natural emissions (dust, sea salt, dimethyl sulfide, biogenic volatile organic compounds (BVOCs) and lightning) and changes in reaction rates for methane and ozone chemistry. The feedback terms are then given by the sensitivity of a pathway to climate change multiplied by the radiative effect of the change.
We find that the overall climate feedback through chemistry and aerosols is negative in the sixth Coupled Model Intercomparison Project (CMIP6) Earth system models due to increased negative forcing from aerosols in a climate with warmer surface temperatures following a quadrupling of CO2 concentrations. This is principally due to increased emissions of sea salt and BVOCs which are sensitive to climate change and cause strong negative radiative forcings. Increased chemical loss of ozone and methane also contributes to a negative feedback. However, overall methane lifetime is expected to increase in a warmer climate due to increased BVOCs. Increased emissions of methane from wetlands would also offset some of the negative feedbacks. The CMIP6 experimental design did not allow the methane lifetime or methane emission changes to affect climate, so we found a robust negative contribution from interactive aerosols and chemistry to climate sensitivity in CMIP6 Earth system models.
Allen, Robert J., Steven T Turnock, Pierre Nabat, David Neubauer, Ülrike Lohmann, Dirk Olivié, Naga Oshima, Martine Michou, Tongwen Wu, J Zhang, Toshihiko Takemura, M Schulz, Kostas Tsigaridis, Susanne E Bauer, Louisa K Emmons, Larry W Horowitz, Vaishali Naik, Twan van Noije, T Bergman, Jean-Francois Lamarque, Prodromos Zanis, I Tegen, Daniel M Westervelt, Philippe Le Sager, Peter Good, Sungbo Shim, Fiona M O'Connor, Dimitris Akritidis, Aristeidis K Georgoulias, Makoto Deushi, Lori T Sentman, Jasmin G John, S Fujimori, and William J Collins, August 2020: Climate and air quality impacts due to mitigation of non-methane near-term climate forcers. Atmospheric Chemistry and Physics, 20(16), DOI:10.5194/acp-20-9641-2020. Abstract
It is important to understand how future environmental policies will impact both climate change and air pollution. Although targeting near-term climate forcers (NTCFs), defined here as aerosols, tropospheric ozone, and precursor gases, should improve air quality, NTCF reductions will also impact climate. Prior assessments of the impact of NTCF mitigation on air quality and climate have been limited. This is related to the idealized nature of some prior studies, simplified treatment of aerosols and chemically reactive gases, as well as a lack of a sufficiently large number of models to quantify model diversity and robust responses. Here, we quantify the 2015–2055 climate and air quality effects of non-methane NTCFs using nine state-of-the-art chemistry–climate model simulations conducted for the Aerosol and Chemistry Model Intercomparison Project (AerChemMIP). Simulations are driven by two future scenarios featuring similar increases in greenhouse gases (GHGs) but with “weak” (SSP3-7.0) versus “strong” (SSP3-7.0-lowNTCF) levels of air quality control measures. As SSP3-7.0 lacks climate policy and has the highest levels of NTCFs, our results (e.g., surface warming) represent an upper bound. Unsurprisingly, we find significant improvements in air quality under NTCF mitigation (strong versus weak air quality controls). Surface fine particulate matter (PM2.5) and ozone (O3) decrease by −2.2±0.32 µg m−3 and −4.6±0.88 ppb, respectively (changes quoted here are for the entire 2015–2055 time period; uncertainty represents the 95 % confidence interval), over global land surfaces, with larger reductions in some regions including south and southeast Asia. Non-methane NTCF mitigation, however, leads to additional climate change due to the removal of aerosol which causes a net warming effect, including global mean surface temperature and precipitation increases of 0.25±0.12 K and 0.03±0.012 mm d−1, respectively. Similarly, increases in extreme weather indices, including the hottest and wettest days, also occur. Regionally, the largest warming and wetting occurs over Asia, including central and north Asia (0.66±0.20 K and 0.03±0.02 mm d−1), south Asia (0.47±0.16 K and 0.17±0.09 mm d−1), and east Asia (0.46±0.20 K and 0.15±0.06 mm d−1). Relatively large warming and wetting of the Arctic also occur at 0.59±0.36 K and 0.04±0.02 mm d−1, respectively. Similar surface warming occurs in model simulations with aerosol-only mitigation, implying weak cooling due to ozone reductions. Our findings suggest that future policies that aggressively target non-methane NTCF reductions will improve air quality but will lead to additional surface warming, particularly in Asia and the Arctic. Policies that address other NTCFs including methane, as well as carbon dioxide emissions, must also be adopted to meet climate mitigation goals.
Archibald, Alexander T., Jessica L Neu, Yasin F Elshorbany, Owen R Cooper, Paul J Young, Hideharu Akiyoshi, R A Cox, Mhairi Coyle, Richard G Derwent, Makoto Deushi, Angelo Finco, Gregory J Frost, Ian E Galbally, Giacomo Gerosa, Claire Granier, Paul T Griffiths, Ryan Hossaini, Lu Hu, Patrick Jöckel, Beatrice Josse, Meiyun Lin, Mariano Mertens, Olaf Morgenstern, Manish Naja, and Vaishali Naik, et al., December 2020: Tropospheric ozone assessment report: A critical review of changes in the tropospheric ozone burden and budget from 1850 to 2100. Elementa: Science of the Anthropocene, 8(1), DOI:10.1525/elementa.2020.034. Abstract
Our understanding of the processes that control the burden and budget of tropospheric ozone has changed dramatically over the last 60 years. Models are the key tools used to understand these changes, and these underscore that there are many processes important in controlling the tropospheric ozone budget. In this critical review, we assess our evolving understanding of these processes, both physical and chemical. We review model simulations from the International Global Atmospheric Chemistry Atmospheric Chemistry and Climate Model Intercomparison Project and Chemistry Climate Modelling Initiative to assess the changes in the tropospheric ozone burden and its budget from 1850 to 2010. Analysis of these data indicates that there has been significant growth in the ozone burden from 1850 to 2000 (approximately 43 ± 9%) but smaller growth between 1960 and 2000 (approximately 16 ± 10%) and that the models simulate burdens of ozone well within recent satellite estimates. The Chemistry Climate Modelling Initiative model ozone budgets indicate that the net chemical production of ozone in the troposphere plateaued in the 1990s and has not changed since then inspite of increases in the burden. There has been a shift in net ozone production in the troposphere being greatest in the northern mid and high latitudes to the northern tropics, driven by the regional evolution of precursor emissions. An analysis of the evolution of tropospheric ozone through the 21st century, as simulated by Climate Model Intercomparison Project Phase 5 models, reveals a large source of uncertainty associated with models themselves (i.e., in the way that they simulate the chemical and physical processes that control tropospheric ozone). This structural uncertainty is greatest in the near term (two to three decades), but emissions scenarios dominate uncertainty in the longer term (2050–2100) evolution of tropospheric ozone. This intrinsic model uncertainty prevents robust predictions of near-term changes in the tropospheric ozone burden, and we review how progress can be made to reduce this limitation.
We document the development and simulation characteristics of the next generation modeling system for seasonal to decadal prediction and projection at the Geophysical Fluid Dynamics Laboratory (GFDL). SPEAR (Seamless System for Prediction and EArth System Research) is built from component models recently developed at GFDL ‐ the AM4 atmosphere model, MOM6 ocean code, LM4 land model and SIS2 sea ice model. The SPEAR models are specifically designed with attributes needed for a prediction model for seasonal to decadal time scales, including the ability to run large ensembles of simulations with available computational resources. For computational speed SPEAR uses a coarse ocean resolution of approximately 1.0o (with tropical refinement). SPEAR can use differing atmospheric horizontal resolutions ranging from 1o to 0.25o. The higher atmospheric resolution facilitates improved simulation of regional climate and extremes. SPEAR is built from the same components as the GFDL CM4 and ESM 4 models, but with design choices geared toward seasonal to multidecadal physical climate prediction and projection. We document simulation characteristics for the time‐mean climate, aspects of internal variability, and the response to both idealized and realistic radiative forcing change. We describe in greater detail one focus of the model development process that was motivated by the importance of the Southern Ocean to the global climate system. We present sensitivity tests that document the influence of the Antarctic surface heat budget on Southern Ocean ventilation and deep global ocean circulation. These findings were also useful in the development processes for the GFDL CM4 and ESM 4 models.
We describe the baseline coupled model configuration and simulation characteristics of GFDL's Earth System Model Version 4.1 (ESM4.1), which builds on component and coupled model developments at GFDL over 2013–2018 for coupled carbon‐chemistry‐climate simulation contributing to the sixth phase of the Coupled Model Intercomparison Project. In contrast with GFDL's CM4.0 development effort that focuses on ocean resolution for physical climate, ESM4.1 focuses on comprehensiveness of Earth system interactions. ESM4.1 features doubled horizontal resolution of both atmosphere (2° to 1°) and ocean (1° to 0.5°) relative to GFDL's previous‐generation coupled ESM2‐carbon and CM3‐chemistry models. ESM4.1 brings together key representational advances in CM4.0 dynamics and physics along with those in aerosols and their precursor emissions, land ecosystem vegetation and canopy competition, and multiday fire; ocean ecological and biogeochemical interactions, comprehensive land‐atmosphere‐ocean cycling of CO2, dust and iron, and interactive ocean‐atmosphere nitrogen cycling are described in detail across this volume of JAMES and presented here in terms of the overall coupling and resulting fidelity. ESM4.1 provides much improved fidelity in CO2 and chemistry over ESM2 and CM3, captures most of CM4.0's baseline simulations characteristics, and notably improves on CM4.0 in (1) Southern Ocean mode and intermediate water ventilation, (2) Southern Ocean aerosols, and (3) reduced spurious ocean heat uptake. ESM4.1 has reduced transient and equilibrium climate sensitivity compared to CM4.0. Fidelity concerns include (1) moderate degradation in sea surface temperature biases, (2) degradation in aerosols in some regions, and (3) strong centennial scale climate modulation by Southern Ocean convection.
Changes in atmospheric methane abundance have implications for both chemistry and climate as methane is both a strong greenhouse gas and an important precursor for tropospheric ozone. A better understanding of the drivers of trends and variability in methane abundance over the recent past is therefore critical for building confidence in projections of future methane levels. In this work, the representation of methane in the atmospheric chemistry model AM4.1 is improved by optimizing total methane emissions (to an annual mean of 576 ± 32 Tg yr−1) to match surface observations over 1980–2017. The simulations with optimized global emissions are in general able to capture the observed global trend, variability, seasonal cycle, and latitudinal gradient of methane. Simulations with different emission adjustments suggest that increases in methane sources (mainly from energy and waste sectors) balanced by increases in methane sinks (mainly due to increases in OH levels) lead to methane stabilization (with an imbalance of 5 Tg yr−1) during 1999–2006, and that increases in methane sources combined with little change in sinks (despite small decreases in OH levels) during 2007–2012 lead to renewed methane growth (with an imbalance of 14 Tg yr−1 for 2007–2017). Compared to 1999–2006, both methane emissions and sinks are greater (by 31 Tg yr−1 and 22 Tg yr−1, respectively) during 2007–2017. Our results also indicate that the energy sector is more likely a major contributor to the methane renewed growth after 2006 than wetland, as increases in wetland emissions alone are not able to explain the renewed methane growth with constant anthropogenic emissions. In addition, a significant increase in wetland emissions would be required starting in 2006, if anthropogenic emissions declined, for wetland emissions to drive renewed growth in methane, which is a less likely scenario. Simulations with varying OH levels indicate that 1 % change in OH levels could lead to an annual mean of ~ 4 Tg yr−1 difference in the optimized emissions and 0.08 year difference in the estimated tropospheric methane lifetime. Continued increases in methane emissions along with decreases in tropospheric OH concentrations during 2008–2015 prolong methane lifetime and therefore amplify the response of methane concentrations to emission changes. Uncertainties still exist in the partitioning of emissions among individual sources and regions.
We describe the baseline model configuration and simulation characteristics of the Geophysical Fluid Dynamics Laboratory (GFDL)'s Atmosphere Model version 4.1 (AM4.1), which builds on developments at GFDL over 2013–2018 for coupled carbon‐chemistry‐climate simulation as part of the sixth phase of the Coupled Model Intercomparison Project. In contrast with GFDL's AM4.0 development effort, which focused on physical and aerosol interactions and which is used as the atmospheric component of CM4.0, AM4.1 focuses on comprehensiveness of Earth system interactions. Key features of this model include doubled horizontal resolution of the atmosphere (~200 to ~100 km) with revised dynamics and physics from GFDL's previous‐generation AM3 atmospheric chemistry‐climate model. AM4.1 features improved representation of atmospheric chemical composition, including aerosol and aerosol precursor emissions, key land‐atmosphere interactions, comprehensive land‐atmosphere‐ocean cycling of dust and iron, and interactive ocean‐atmosphere cycling of reactive nitrogen. AM4.1 provides vast improvements in fidelity over AM3, captures most of AM4.0's baseline simulations characteristics, and notably improves on AM4.0 in the representation of aerosols over the Southern Ocean, India, and China—even with its interactive chemistry representation—and in its manifestation of sudden stratospheric warmings in the coldest months. Distributions of reactive nitrogen and sulfur species, carbon monoxide, and ozone are all substantially improved over AM3. Fidelity concerns include degradation of upper atmosphere equatorial winds and of aerosols in some regions.
Morgenstern, Olaf, Fiona M O'Connor, Ben Johnson, Guang Zeng, Jane P Mulcahy, Jonny Williams, João Teixeira, Martine Michou, Pierre Nabat, Larry W Horowitz, Vaishali Naik, and Lori T Sentman, et al., October 2020: Reappraisal of the Climate Impacts of Ozone‐Depleting Substances. Geophysical Research Letters, 47(20), DOI:10.1029/2020GL088295. Abstract
We assess the effective radiative forcing due to ozone‐depleting substances using models participating in the Aerosols and Chemistry and Radiative Forcing Model Intercomparison Projects (AerChemMIP, RFMIP). A large intermodel spread in this globally averaged quantity necessitates an “emergent constraint” approach whereby we link the radiative forcing to ozone declines measured and simulated during 1979–2000, excluding two volcanically perturbed periods. During this period, ozone‐depleting substances were increasing, and several merged satellite‐based climatologies document the ensuing decline of total‐column ozone. Using these analyses, we find an effective radiative forcing of −0.05 to 0.13 W m−2. Our best estimate (0.04 W m−2) is on the edge of the “likely” range given by the Fifth Assessment Report of IPCC of 0.03 to 0.33 W m−2 but is in better agreement with two other literature results.
Peters, Daniel R., Jordan L Schnell, Patrick L Kinney, Vaishali Naik, and Daniel E Horton, October 2020: Public Health and Climate Benefits and Tradeoffs of U.S. Vehicle Electrification. GeoHealth, 4(10), DOI:10.1029/2020GH000275. Abstract
Vehicle electrification is a common climate change mitigation strategy, with policymakers invoking co‐beneficial reductions in carbon dioxide (CO2) and air pollutant emissions. However, while previous studies of U.S. electric vehicle (EV) adoption consistently predict CO2 mitigation benefits, air quality outcomes are equivocal and depend on policies assessed and experimental parameters. We analyze climate and health co‐benefits and trade‐offs of six U.S. EV adoption scenarios: 25% or 75% replacement of conventional internal combustion engine vehicles, each under three different EV‐charging energy generation scenarios. We transfer emissions from tailpipe to power generation plant, simulate interactions of atmospheric chemistry and meteorology using the GFDL‐AM4 chemistry climate model, and assess health consequences and uncertainties using the U.S. Environmental Protection Agency Benefits Mapping Analysis Program Community Edition (BenMAP‐CE). We find that 25% U.S. EV adoption, with added energy demand sourced from the present‐day electric grid, annually results in a ~242 M ton reduction in CO2 emissions, 437 deaths avoided due to PM2.5 reductions (95% CI: 295, 578), and 98 deaths avoided due to lesser ozone formation (95% CI: 33, 162). Despite some regions experiencing adverse health outcomes, ~$16.8B in damages avoided are predicted. Peak CO2 reductions and health benefits occur with 75% EV adoption and increased emission‐free energy sources (~$70B in damages avoided). When charging‐electricity from aggressive EV adoption is combustion‐only, adverse health outcomes increase substantially, highlighting the importance of low‐to‐zero emission power generation for greater realization of health co‐benefits. Our results provide a more nuanced understanding of the transportation sector's climate change mitigation‐health impact relationship.
Dust emission is initiated when surface wind velocities exceed the threshold of wind erosion. Most dust models used constant threshold values globally. Here we use satellite products to characterize the frequency of dust events and surface properties. By matching this frequency derived from Moderate Resolution Imaging Spectroradiometer (MODIS) Deep Blue aerosol products with surface winds, we are able to retrieve a climatological monthly global distribution of wind erosion threshold (Vthreshold) over dry and sparsely-vegetated surface. This monthly two-dimensional threshold velocity is then implemented into the Geophysical Fluid Dynamics Laboratory coupled land-atmosphere model (AM4.0/LM4.0). It is found that the climatology of dust optical depth (DOD) and total aerosol optical depth, surface PM10 dust concentrations, and seasonal cycle of DOD are better captured over the dust belt (i.e. North Africa and the Middle East) by simulations with the new wind erosion threshold than those using the default globally constant threshold. The most significant improvement is the frequency distribution of dust events, which is generally ignored in model evaluation. By using monthly rather than annual mean Vthreshold, all comparisons with observations are further improved. The monthly global threshold of wind erosion can be retrieved under different spatial resolutions to match the resolution of dust models and thus can help improve the simulations of dust climatology and seasonal cycle as well as dust forecasting.
Saunois, Marielle, Ann R Stavert, Ben Poulter, Philippe Bousquet, Josep G Canadell, Robert B Jackson, Peter A Raymond, Edward J Dlugokencky, Sander Houweling, Prabir K Patra, Philippe Ciais, Vivek Arora, David Bastviken, Peter Bergamaschi, Donald R Blake, Gordon Brailsford, Lori Bruhwiler, Kimberly M Carlson, Mark Carrol, Simona Castaldi, Naveen Chandra, Cyril Crevoisier, Patrick Crill, Kristofer Covey, Charles Curry, Giuseppe Etiope, Christian Frankenberg, Nicola Gedney, Michaela I Hegglin, Lena Höglund-Isaksson, Gustaf Hugelius, Misa Ishizawa, Akihiko Ito, Greet Janssens-Manehout, Katherine M Jensen, Fortunat Joos, Thomas Kleinen, Paul Krummel, Ray L Langenfelds, Goulven G Laruelle, Licheng Liu, Toshinobu Machida, Shamil Maksyutov, Kyle C McDonald, Joe McNorton, Paul A Miller, Joe R Melton, Isamu Morino, Jurek Müller, Fabiola Murguia-Flores, and Vaishali Naik, et al., July 2020: The Global Methane Budget 2000–2017. Earth System Science Data, 12(3), DOI:10.5194/essd-12-1561-2020. Abstract
Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH4 continue to increase, making CH4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO2). The relative importance of CH4 compared to CO2 depends on its shorter atmospheric lifetime, stronger warming potential, and variations in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the atmospheric growth rate arise from the variety of geographically overlapping CH4 sources and from the destruction of CH4 by short-lived hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations).
Stevenson, David S., Alcide Zhao, Vaishali Naik, Fiona M O'Connor, Simone Tilmes, Guang Zeng, Lee T Murray, William J Collins, Paul T Griffiths, Sungbo Shim, Larry W Horowitz, Lori T Sentman, and Louisa K Emmons, November 2020: Trends in global tropospheric hydroxyl radical and methane lifetime since 1850 from AerChemMIP. Atmospheric Chemistry and Physics, 20(21), DOI:10.5194/acp-20-12905-2020. Abstract
We analyse historical (1850–2014) atmospheric hydroxyl (OH) and methane lifetime data from Coupled Model Intercomparison Project Phase 6 (CMIP6)/Aerosols and Chemistry Model Intercomparison Project (AerChemMIP) simulations. Tropospheric OH changed little from 1850 up to around 1980, then increased by around 9 % up to 2014, with an associated reduction in methane lifetime. The model-derived OH trends from 1980 to 2005 are broadly consistent with trends estimated by several studies that infer OH from inversions of methyl chloroform and associated measurements; most inversion studies indicate decreases in OH since 2005. However, the model results fall within observational uncertainty ranges. The upward trend in modelled OH since 1980 was mainly driven by changes in anthropogenic near-term climate forcer emissions (increases in anthropogenic nitrogen oxides and decreases in CO). Increases in halocarbon emissions since 1950 have made a small contribution to the increase in OH, whilst increases in aerosol-related emissions have slightly reduced OH. Halocarbon emissions have dramatically reduced the stratospheric methane lifetime by about 15 %–40 %; most previous studies assumed a fixed stratospheric lifetime. Whilst the main driver of atmospheric methane increases since 1850 is emissions of methane itself, increased ozone precursor emissions have significantly modulated (in general reduced) methane trends. Halocarbon and aerosol emissions are found to have relatively small contributions to methane trends. These experiments do not isolate the effects of climate change on OH and methane evolution; however, we calculate residual terms that are due to the combined effects of climate change and non-linear interactions between drivers. These residual terms indicate that non-linear interactions are important and differ between the two methodologies we use for quantifying OH and methane drivers. All these factors need to be considered in order to fully explain OH and methane trends since 1850; these factors will also be important for future trends.
Turnock, Steven T., Robert J Allen, Martin Andrews, Susanne E Bauer, Louisa K Emmons, Peter Good, Larry W Horowitz, Jasmin G John, Martine Michou, Pierre Nabat, and Vaishali Naik, et al., November 2020: Historical and future changes in air pollutants from CMIP6 models. Atmospheric Chemistry and Physics, 20(23), DOI:10.5194/acp-20-14547-2020. Abstract
Poor air quality is currently responsible for large impacts on human health across the world. In addition, the air pollutants ozone (O3) and particulate matter less than 2.5 µm in diameter (PM2.5) are also radiatively active in the atmosphere and can influence Earth's climate. It is important to understand the effect of air quality and climate mitigation measures over the historical period and in different future scenarios to ascertain any impacts from air pollutants on both climate and human health. The Coupled Model Intercomparison Project Phase 6 (CMIP6) presents an opportunity to analyse the change in air pollutants simulated by the current generation of climate and Earth system models that include a representation of chemistry and aerosols (particulate matter). The shared socio-economic pathways (SSPs) used within CMIP6 encompass a wide range of trajectories in precursor emissions and climate change, allowing for an improved analysis of future changes to air pollutants. Firstly, we conduct an evaluation of the available CMIP6 models against surface observations of O3 and PM2.5. CMIP6 models consistently overestimate observed surface O3 concentrations across most regions and in most seasons by up to 16 ppb, with a large diversity in simulated values over Northern Hemisphere continental regions. Conversely, observed surface PM2.5 concentrations are consistently underestimated in CMIP6 models by up to 10 µg m−3, particularly for the Northern Hemisphere winter months, with the largest model diversity near natural emission source regions. The biases in CMIP6 models when compared to observations of O3 and PM2.5 are similar to those found in previous studies. Over the historical period (1850–2014) large increases in both surface O3 and PM2.5 are simulated by the CMIP6 models across all regions, particularly over the mid to late 20th century, when anthropogenic emissions increase markedly. Large regional historical changes are simulated for both pollutants across East and South Asia with an annual mean increase of up to 40 ppb for O3 and 12 µg m−3 for PM2.5. In future scenarios containing strong air quality and climate mitigation measures (ssp126), annual mean concentrations of air pollutants are substantially reduced across all regions by up to 15 ppb for O3 and 12 µg m−3 for PM2.5. However, for scenarios that encompass weak action on mitigating climate and reducing air pollutant emissions (ssp370), annual mean increases in both surface O3 (up 10 ppb) and PM2.5 (up to 8 µg m−3) are simulated across most regions, although, for regions like North America and Europe small reductions in PM2.5 are simulated due to the regional reduction in precursor emissions in this scenario. A comparison of simulated regional changes in both surface O3 and PM2.5 from individual CMIP6 models highlights important regional differences due to the simulated interaction of aerosols, chemistry, climate and natural emission sources within models. The projection of regional air pollutant concentrations from the latest climate and Earth system models used within CMIP6 shows that the particular future trajectory of climate and air quality mitigation measures could have important consequences for regional air quality, human health and near-term climate. Differences between individual models emphasise the importance of understanding how future Earth system feedbacks influence natural emission sources, e.g. response of biogenic emissions under climate change.
We describe GFDL's CM4.0 physical climate model, with emphasis on those aspects that may be of particular importance to users of this model and its simulations. The model is built with the AM4.0/LM4.0 atmosphere/land model and OM4.0 ocean model. Topics include the rationale for key choices made in the model formulation, the stability as well as drift of the pre‐industrial control simulation, and comparison of key aspects of the historical simulations with observations from recent decades. Notable achievements include the relatively small biases in seasonal spatial patterns of top‐of‐atmosphere fluxes, surface temperature, and precipitation; reduced double Intertropical Convergence Zone bias; dramatically improved representation of ocean boundary currents; a high quality simulation of climatological Arctic sea ice extent and its recent decline; and excellent simulation of the El Niño‐Southern Oscillation spectrum and structure. Areas of concern include inadequate deep convection in the Nordic Seas; an inaccurate Antarctic sea ice simulation; precipitation and wind composites still affected by the equatorial cold tongue bias; muted variability in the Atlantic Meridional Overturning Circulation; strong 100 year quasi‐periodicity in Southern Ocean ventilation; and a lack of historical warming before 1990 and too rapid warming thereafter due to high climate sensitivity and strong aerosol forcing, in contrast to the observational record. Overall, CM4.0 scores very well in its fidelity against observations compared to the Coupled Model Intercomparison Project Phase 5 generation in terms of both mean state and modes of variability and should prove a valuable new addition for analysis across a broad array of applications.
Black carbon (BC) mitigation can reduce adverse environmental impacts on climate, air quality, human health, and water resource availability. To facilitate the identification of mitigation priorities, we use a state-of-the-science global chemistry-climate coupled model (AM3), with additional tagged BC tracers representing regional (East Asia, South Asia, Europe and North America) and sectoral (land transport, residential, industry) anthropogenic BC emissions to identify sources with the largest impacts on air quality, human health and glacial deposition. We find that within each tagged region, domestic emissions dominate BC surface concentrations and associated premature mortality (generally over 90%), as well as BC deposition on glaciers (∼40–95% across glaciers). BC emissions occurring within each tagged source region contribute roughly 1–2 orders of magnitude more to their domestic BC concentrations, premature mortality, and BC deposition on regional glaciers than that caused by the same quantity of BC emitted from foreign regions. At the sectoral level, the South Asian residential sector contributes ∼60% of BC associated premature mortality in South Asia and ∼40–60% of total BC deposited on southern Tibetan glaciers. Our findings imply that BC mitigation within a source region, particularly from East and South Asian residential sectors, will bring the largest reductions in BC associated air pollution, premature mortality, and glacial deposition.
Ramaswamy, V, William D Collins, Jim M Haywood, J Lean, Natalie M. Mahowald, Gunnar Myhre, and Vaishali Naik, et al., November 2019: Radiative Forcing of Climate: The Historical Evolution of the Radiative Forcing Concept, the Forcing Agents and their Quantification, and Applications In A Century of Progress in Atmospheric and Related Sciences: Celebrating the American Meteorological Society Centennial, Boston, MA, Meteorological Monographs, American Meteorological Society, 59, DOI:10.1175/AMSMONOGRAPHS-D-19-0001.114.1-14.100. Abstract
We describe the historical evolution of the conceptualization, formulation, quantification, application, and utilization of “radiative forcing” (RF) of Earth’s climate. Basic theories of shortwave and longwave radiation were developed through the nineteenth and twentieth centuries and established the analytical framework for defining and quantifying the perturbations to Earth’s radiative energy balance by natural and anthropogenic influences. The insight that Earth’s climate could be radiatively forced by changes in carbon dioxide, first introduced in the nineteenth century, gained empirical support with sustained observations of the atmospheric concentrations of the gas beginning in 1957. Advances in laboratory and field measurements, theory, instrumentation, computational technology, data, and analysis of well-mixed greenhouse gases and the global climate system through the twentieth century enabled the development and formalism of RF; this allowed RF to be related to changes in global-mean surface temperature with the aid of increasingly sophisticated models. This in turn led to RF becoming firmly established as a principal concept in climate science by 1990. The linkage with surface temperature has proven to be the most important application of the RF concept, enabling a simple metric to evaluate the relative climate impacts of different agents. The late 1970s and 1980s saw accelerated developments in quantification, including the first assessment of the effect of the forcing due to the doubling of carbon dioxide on climate (the “Charney” report). The concept was subsequently extended to a wide variety of agents beyond well-mixed greenhouse gases (WMGHGs; carbon dioxide, methane, nitrous oxide, and halocarbons) to short-lived species such as ozone. The WMO and IPCC international assessments began the important sequence of periodic evaluations and quantifications of the forcings by natural (solar irradiance changes and stratospheric aerosols resulting from volcanic eruptions) and a growing set of anthropogenic agents (WMGHGs, ozone, aerosols, land surface changes, contrails). From the 1990s to the present, knowledge and scientific confidence in the radiative agents acting on the climate system have proliferated. The conceptual basis of RF has also evolved as both our understanding of the way radiative forcing drives climate change and the diversity of the forcing mechanisms have grown. This has led to the current situation where “effective radiative forcing” (ERF) is regarded as the preferred practical definition of radiative forcing in order to better capture the link between forcing and global-mean surface temperature change. The use of ERF, however, comes with its own attendant issues, including challenges in its diagnosis from climate models, its applications to small forcings, and blurring of the distinction between rapid climate adjustments (fast responses) and climate feedbacks; this will necessitate further elaboration of its utility in the future. Global climate model simulations of radiative perturbations by various agents have established how the forcings affect other climate variables besides temperature (e.g., precipitation). The forcing–response linkage as simulated by models, including the diversity in the spatial distribution of forcings by the different agents, has provided a practical demonstration of the effectiveness of agents in perturbing the radiative energy balance and causing climate changes. The significant advances over the past half century have established, with very high confidence, that the global-mean ERF due to human activity since preindustrial times is positive (the 2013 IPCC assessment gives a best estimate of 2.3 W m−2, with a range from 1.1 to 3.3 W m−2; 90% confidence interval). Further, except in the immediate aftermath of climatically significant volcanic eruptions, the net anthropogenic forcing dominates over natural radiative forcing mechanisms. Nevertheless, the substantial remaining uncertainty in the net anthropogenic ERF leads to large uncertainties in estimates of climate sensitivity from observations and in predicting future climate impacts. The uncertainty in the ERF arises principally from the incorporation of the rapid climate adjustments in the formulation, the well-recognized difficulties in characterizing the preindustrial state of the atmosphere, and the incomplete knowledge of the interactions of aerosols with clouds. This uncertainty impairs the quantitative evaluation of climate adaptation and mitigation pathways in the future. A grand challenge in Earth system science lies in continuing to sustain the relatively simple essence of the radiative forcing concept in a form similar to that originally devised, and at the same time improving the quantification of the forcing. This, in turn, demands an accurate, yet increasingly complex and comprehensive, accounting of the relevant processes in the climate system.
A central strategy in achieving greenhouse gas mitigation targets is the transition of vehicles from internal combustion engines to electric power. However, due to complex emission sources and nonlinear chemistry, it is unclear how such a shift might impact air quality. Here we apply a prototype version of the new-generation NOAA GFDL global Atmospheric Model, version 4 (GFDL AM4) to investigate the impact on U.S. air quality from an aggressive conversion of internal combustion vehicles to battery-powered electric vehicles (EVs). We examine a suite of scenarios designed to quantify the effect of both the magnitude of EV market penetration and the source of electricity generation used to power them. We find that summer surface ozone (O3) decreases in most locations due to widespread reductions of traffic NOx emissions. Summer fine particulate matter (PM2.5) increases on average and largest in areas with increased coal-fired power generation demands. Winter O3 increases due to reduced loss via traffic NOx while PM2.5 decreases since larger ammonium nitrate reductions offset increases in ammonium sulfate. The largest magnitude changes are simulated at the extremes of the probability distribution. Increasing the fraction of vehicles converted to EVs further decreases summer O3, while increasing the fraction of electricity generated by “emission-free” sources largely eliminates the increases in summer PM2.5 at high EV adoption fractions. Ultimately, the number of conventional vehicles replaced by EVs has a larger effect on O3 than PM2.5, while the source of the electricity for those EVs exhibit greater control on PM2.5.
Derwent, Richard G., David D Parrish, Ian E Galbally, David S Stevenson, R Doherty, Vaishali Naik, and Paul J Young, May 2018: Uncertainties in models of tropospheric ozone based on Monte Carlo analysis: Tropospheric ozone burdens, atmospheric lifetimes and surface distributions. Atmospheric Environment, 180, DOI:10.1016/j.atmosenv.2018.02.047. Abstract
Recognising that global tropospheric ozone models have many uncertain input parameters, an attempt has been made to employ Monte Carlo sampling to quantify the uncertainties in model output that arise from global tropospheric ozone precursor emissions and from ozone production and destruction in a global Lagrangian chemistry-transport model. Ninety eight quasi-randomly Monte Carlo sampled model runs were completed and the uncertainties were quantified in tropospheric burdens and lifetimes of ozone, carbon monoxide and methane, together with the surface distribution and seasonal cycle in ozone. The results have shown a satisfactory degree of convergence and provide a first estimate of the likely uncertainties in tropospheric ozone model outputs. There are likely to be diminishing returns in carrying out many more Monte Carlo runs in order to refine further these outputs. Uncertainties due to model formulation were separately addressed using the results from 14 Atmospheric Chemistry Coupled Climate Model Intercomparison Project (ACCMIP) chemistry-climate models. The 95% confidence ranges surrounding the ACCMIP model burdens and lifetimes for ozone, carbon monoxide and methane were somewhat smaller than for the Monte Carlo estimates. This reflected the situation where the ACCMIP models used harmonised emissions data and differed only in their meteorological data and model formulations whereas a conscious effort was made to describe the uncertainties in the ozone precursor emissions and in the kinetic and photochemical data in the Monte Carlo runs. Attention was focussed on the model predictions of the ozone seasonal cycles at three marine boundary layer stations: Mace Head, Ireland, Trinidad Head, California and Cape Grim, Tasmania. Despite comprehensively addressing the uncertainties due to global emissions and ozone sources and sinks, none of the Monte Carlo runs were able to generate seasonal cycles that matched the observations at all three MBL stations. Although the observed seasonal cycles were found to fall within the confidence limits of the ACCMIP members, this was because the model seasonal cycles spanned extremely wide ranges and there was no single ACCMIP member that performed best for each station. Further work is required to examine the parameterisation of convective mixing in the models to see if this erodes the isolation of the marine boundary layer from the free troposphere and thus hides the models' real ability to reproduce ozone seasonal cycles over marine stations.
Lefohn, A S., C S Malley, L Smith, B Wells, M Hazucha, H Simon, and Vaishali Naik, et al., April 2018: Tropospheric ozone assessment report: Global ozone metrics for climate change, human health, and crop/ecosystem research. Elementa: Science of the Anthropocene, 6(1), 28, DOI:10.1525/elementa.279. Abstract
Assessment of spatial and temporal variation in the impacts of ozone on human health, vegetation, and climate requires appropriate metrics. A key component of the Tropospheric Ozone Assessment Report (TOAR) is the consistent calculation of these metrics at thousands of monitoring sites globally. Investigating temporal trends in these metrics required that the same statistical methods be applied across these ozone monitoring sites. The nonparametric Mann-Kendall test (for significant trends) and the Theil-Sen estimator (for estimating the magnitude of trend) were selected to provide robust methods across all sites. This paper provides the scientific underpinnings necessary to better understand the implications of and rationale for selecting a specific TOAR metric for assessing spatial and temporal variation in ozone for a particular impact. The rationale and underlying research evidence that influence the derivation of specific metrics are given. The form of 25 metrics (4 for model-measurement comparison, 5 for characterization of ozone in the free troposphere, 11 for human health impacts, and 5 for vegetation impacts) are described. Finally, this study categorizes health and vegetation exposure metrics based on the extent to which they are determined only by the highest hourly ozone levels, or by a wider range of values. The magnitude of the metrics is influenced by both the distribution of hourly average ozone concentrations at a site location, and the extent to which a particular metric is determined by relatively low, moderate, and high hourly ozone levels. Hence, for the same ozone time series, changes in the distribution of ozone concentrations can result in different changes in the magnitude and direction of trends for different metrics. Thus, dissimilar conclusions about the effect of changes in the drivers of ozone variability (e.g., precursor emissions) on health and vegetation exposure can result from the selection of different metrics.
Nolte, Christopher G., Patrick D Dolwick, Neal Fann, Larry W Horowitz, and Vaishali Naik, et al., 2018: Air Quality In Impacts, Risks, and Adaptation in the United States: Fourth National Climate Assessment, Volume II [Reidmiller, D.R., C.W. Avery, D.R. Easterling, K.E. Kunkel, K.L.M. Lewis, T.K. Maycock, and B.C. Stewart (eds.)], Washington, DC, USA, U.S. Global Change Research Program, DOI:10.7930/NCA4.2018.CH13512-538.
It is clear that the most effective way to limit global temperature rise and associated impacts is to reduce human emissions of greenhouse gases, including methane. However, quantification of the climate benefits of mitigation options are complicated by the contrast in the timescales at which short-lived climate pollutants, such as methane, persist in the atmosphere as compared to carbon dioxide. Whereas simple metrics fail to capture the differential impacts across all timescales, sophisticated climate models that can address these temporal dynamics are often inaccessible, time-intensive, and require special infrastructure. Reduced-complexity models offer an ideal compromise in that they provide quick, reliable insights into the benefits across types of climate pollutants using basic knowledge and limited computational infrastructure. In this paper, we build on previous evaluations of the freely-available and easy-to-run reduced-complexity climate model MAGICC by confirming its ability to reproduce temperature responses to historical methane emissions. By comparing MAGICC model results to those from the reference GFDL CM3 coupled global chemistry-climate model, we build confidence in using MAGICC for purposes of understanding the climate implications of methane mitigation. MAGICC can easily and rapidly provide robust data on climate responses to changes in methane emissions.
We present observation and model-based estimates of the changes in the direct shortwave effect of aerosols under clear-sky (SDRECS) from 2001 to 2015. Observation-based estimates are obtained from changes in the outgoing shortwave clear-sky radiation (Rsutcs) measured by the Clouds and the Earth's Radiant Energy System (CERES), accounting for the effect of variability in surface albedo, water vapor, and ozone. We find increases in SDRECS (i.e., less radiation scattered to space by aerosols) over Western Europe (0.7–1 W m−2 dec−1) and the Eastern US (0.9–1.8 W m−2 dec−1), decreases over India (−0.5– −1.9 W m−2 dec−1) and no significant change over Eastern China. Comparisons with the GFDL chemistry climate model AM3, driven by CMIP6 historical emissions, show that changes in SDRECS over Western Europe and the Eastern US are well captured, which largely reflects the mature understanding of the sulfate budget in these regions. In contrast, the model overestimates the trends in SDRECS over India and Eastern China. Over China, this bias can be partly attributed to the decline of SO2 emissions after 2007, which is not captured by the CMIP6 emissions. In both India and Eastern China, we find much larger contributions of nitrate and black carbon to changes in SDRECS than in the US and Europe, which highlights the need to better constrain their precursors and chemistry. Globally, our model shows that changes in the all-sky aerosol direct forcing between 2001 and 2015 (+0.03 W m−2) are dominated by black carbon (+0.12 W m−2) with significant offsets from nitrate (−0.03 W m−2) and sulfate (−0.03 W m−2). Changes in the sulfate (+7 %) and nitrate (+60 %) all-sky direct forcing between 2001 and 2015 are only weakly related to changes in the emissions of their precursors (−12.5 % and 19 % for SO2 and NH3, respectively), due mostly to chemical non linearities.
Rieder, H E., Arlene M Fiore, Olivia E Clifton, G Correa, Larry W Horowitz, and Vaishali Naik, November 2018: Combining model projections with site-level observations to estimate changes in distributions and seasonality of ozone in surface air over the USA. Atmospheric Environment, 193, DOI:10.1016/j.atmosenv.2018.07.042. Abstract
While compliance with air quality standards is evaluated at individual monitoring stations, projections of future ambient air quality for global climate and emission scenarios often rely on coarse resolution models. We describe a statistical transfer approach that bridges the spatial gap between air quality projections, averaged over four broad U.S. regions, from a global chemistry-climate model and the local level (at specific U.S. CASTNet sites). Our site-level projections are intended as a line of evidence in planning for possible futures rather than the sole basis for policy decisions. We use a set of transient sensitivity simulations (2006–2100) from the Geophysical Fluid Dynamics Laboratory (GFDL) chemistry-climate model CM3, designed to isolate the effects of changes in anthropogenic ozone (O3) precursor emissions, climate warming, and global background CH4 on surface O3. We find that surface maximum daily 8-h average (MDA8) O3 increases despite constant precursor emissions in a warmer climate during summer, particularly in the low tail of the MDA8 O3 distribution for the Northeastern U.S., while MDA8 O3 decreases slightly throughout the distribution over the West and Southeast during summer and fall. Under scenarios in which non-methane O3 precursors decline as climate warms (RCP4.5 and RCP8.5), summertime MDA8 O3 decreases with NOx emissions, most strongly in the upper tail of the MDA8 O3 distribution. In a scenario where global methane abundances roughly double over the 21st century (RCP8.5), winter and spring MDA8 O3 increases, particularly in the lower tail and over the Western U.S. In this RCP8.5 scenario, the number of days when MDA8 O3 exceeds 70 ppb declines in summer with NOx emissions, but increases in spring (and winter); by the end of the century, the majority of sites in the WE and NE show probabilistic return values of the annual 4th highest MDA8 O3 concentration above 70 ppb (the current O3 NAAQS level). Continued increases in global CH4 abundances can be thought of as a “methane penalty”, offsetting benefits otherwise attainable by controlling non-CH4 O3 precursors.
Northern India (23° N–31° N, 68° E–90° E) is one of the most densely populated and polluted regions in world. Accurately modeling pollution in the region is difficult due to the extreme conditions with respect to emissions, meteorology, and topography, but it is paramount in order to understand how future changes in emissions and climate may alter the region's pollution regime. We evaluate the ability of a developmental version of the new-generation NOAA GFDL Atmospheric Model, version 4 (AM4) to simulate observed wintertime fine particulate matter (PM2.5) and its relationship to meteorology over Northern India. We compare two simulations of GFDL-AM4 nudged to observed meteorology for the period 1980–2016 driven by pollutant emissions from two global inventories developed in support of the Coupled Model Intercomparison Project Phases 5 (CMIP5) and 6 (CMIP6), and compare results with ground-based observations from India's Central Pollution Control Board (CPCB) for the period 1 October 2015–31 March 2016. Overall, our results indicate that the simulation with CMIP6 emissions, produces improved concentrations of pollutants over the region relative to the CMIP5-driven simulation.
While the particulate concentrations simulated by AM4 are biased low overall, the model generally simulates the magnitude and daily variability of observed total PM2.5. Nitrate and organic matter are the primary components of PM2.5 over Northern India in the model. On the basis of correlations of the individual model components with total observed PM2.5 and correlations between the two simulations, meteorology is the primary driver of daily variability. The model correctly reproduces the shape and magnitude of the seasonal cycle of PM2.5, but the simulated diurnal cycle misses the early evening rise and secondary maximum found in the observations. Observed PM2.5 abundances are by far the highest within the densely populated Indo-Gangetic Plain, where they are closely related to boundary layer meteorology, specifically relative humidity, wind speed, boundary layer height, and inversion strength. The GFDL AM4 model reproduces the overall observed pollution gradient over Northern India as well as the strength of the meteorology-PM2.5 relationship in most locations.
Turner, A J., I Y Fung, Vaishali Naik, Larry W Horowitz, and R C Cohen, September 2018: Modulation of hydroxyl variability by ENSO in the absence of external forcing. Proceedings of the National Academy of Sciences, 115(36), DOI:10.1073/pnas.1807532115. Abstract
The hydroxyl radical (OH) is the primary oxidant in the troposphere, and the impact of its fluctuations on the methane budget has been disputed in recent years, however measurements of OH are insufficient to characterize global interannual fluctuations relevant for methane. Here, we use a 6,000-y control simulation of preindustrial conditions with a chemistry-climate model to quantify the natural variability in OH and internal feedbacks governing that variability. We find that, even in the absence of external forcing, maximum OH changes are 3.8 ± 0.8% over a decade, which is large in the context of the recent methane growth from 2007–2017. We show that the OH variability is not a white-noise process. A wavelet analysis indicates that OH variability exhibits significant feedbacks with the same periodicity as the El Niño–Southern Oscillation (ENSO). We find intrinsically generated modulation of the OH variability, suggesting that OH may show periods of rapid or no change in future decades that are solely due to the internal climate dynamics (as opposed to external forcings). An empirical orthogonal function analysis further indicates that ENSO is the dominant mode of OH variability, with the modulation of OH occurring primarily through lightning NOx. La Niña is associated with an increase in convection in the Tropical Pacific, which increases the simulated occurrence of lightning and allows for more OH production. Understanding this link between OH and ENSO may improve the predictability of the oxidative capacity of the troposphere and assist in elucidating the causes of current and historical trends in methane.
Young, Paul J., Vaishali Naik, Arlene M Fiore, Audrey Gaudel, Jean J Guo, and Meiyun Lin, et al., January 2018: Tropospheric Ozone Assessment Report: Assessment of global-scale model performance for global and regional ozone distributions, variability, and trends. Elementa: Science of the Anthropocene, 6(1), 10, DOI:10.1525/elementa.265. Abstract
The goal of the Tropospheric Ozone Assessment Report (TOAR) is to provide the research community with an up-to-date scientific assessment of tropospheric ozone, from the surface to the tropopause. While a suite of observations provides significant information on the spatial and temporal distribution of tropospheric ozone, observational gaps make it necessary to use global atmospheric chemistry models to synthesize our understanding of the processes and variables that control tropospheric ozone abundance and its variability. Models facilitate the interpretation of the observations and allow us to make projections of future tropospheric ozone and trace gas distributions for different anthropogenic or natural perturbations. This paper assesses the skill of current-generation global atmospheric chemistry models in simulating the observed present-day tropospheric ozone distribution, variability, and trends. Drawing upon the results of recent international multi-model intercomparisons and using a range of model evaluation techniques, we demonstrate that global chemistry models are broadly skillful in capturing the spatio-temporal variations of tropospheric ozone over the seasonal cycle, for extreme pollution episodes, and changes over interannual to decadal periods. However, models are consistently biased high in the northern hemisphere and biased low in the southern hemisphere, throughout the depth of the troposphere, and are unable to replicate particular metrics that define the longer term trends in tropospheric ozone as derived from some background sites. When the models compare unfavorably against observations, we discuss the potential causes of model biases and propose directions for future developments, including improved evaluations that may be able to better diagnose the root cause of the model-observation disparity. Overall, model results should be approached critically, including determining whether the model performance is acceptable for the problem being addressed, whether biases can be tolerated or corrected, whether the model is appropriately constituted, and whether there is a way to satisfactorily quantify the uncertainty.
In this two-part paper, a description is provided of a version of the AM4.0/LM4.0 atmosphere/land model that will serve as a base for a new set of climate and Earth system models (CM4 and ESM4) under development at NOAA's Geophysical Fluid Dynamics Laboratory (GFDL). This version, with roughly 100km horizontal resolution and 33 levels in the vertical, contains an aerosol model that generates aerosol fields from emissions and a “light” chemistry mechanism designed to support the aerosol model but with prescribed ozone. In Part I, the quality of the simulation in AMIP (Atmospheric Model Intercomparison Project) mode – with prescribed sea surface temperatures (SSTs) and sea ice distribution – is described and compared with previous GFDL models and with the CMIP5 archive of AMIP simulations. The model's Cess sensitivity (response in the top-of-atmosphere radiative flux to uniform warming of SSTs) and effective radiative forcing are also presented. In Part II, the model formulation is described more fully and key sensitivities to aspects of the model formulation are discussed, along with the approach to model tuning.
In Part II of this two-part paper, documentation is provided of key aspects of a version of the AM4.0/LM4.0 atmosphere/land model that will serve as a base for a new set of climate and Earth system models (CM4 and ESM4) under development at NOAA's Geophysical Fluid Dynamics Laboratory (GFDL). The quality of the simulation in AMIP (Atmospheric Model Intercomparison Project) mode has been provided in Part I. Part II provides documentation of key components and some sensitivities to choices of model formulation and values of parameters, highlighting the convection parameterization and orographic gravity wave drag. The approach taken to tune the model's clouds to observations is a particular focal point. Care is taken to describe the extent to which aerosol effective forcing and Cess sensitivity have been tuned through the model development process, both of which are relevant to the ability of the model to simulate the evolution of temperatures over the last century when coupled to an ocean model.
We use transient GFDL-CM3 chemistry-climate model simulations over the 2006-2100 period to show how the influence of volcanic aerosols on the extent and timing of ozone recovery varies with a) future greenhouse gas scenarios (RCP4.5 and RCP8.5) and b) halogen loading. Current understanding is that elevated volcanic aerosols reduce ozone under high halogen loading, but increase ozone under low halogen loading when the chemistry is more NOx dominated. With extremely low aerosol loadings (designated here as ‘background’), global stratospheric ozone burden is simulated to return to 1980 levels around 2050 in the RCP8.5 scenario, but remains below 1980 levels throughout the 21st century in the RCP4.5 scenario. In contrast, with elevated volcanic aerosols, ozone column recovers more quickly to 1980 levels, with recovery dates ranging from the mid-2040s in RCP8.5 to the mid-2050s to early 2070s in RCP4.5. The ozone response in both future emission scenarios increases with enhanced volcanic aerosols. By 2100, the 1980-baseline adjusted global stratospheric ozone column is projected to be 20-40% greater in RCP8.5 and 110-200% greater in RCP4.5 with elevated volcanic aerosols compared to simulations with the extremely low background aerosols. The weaker ozone enhancement at 2100 in RCP8.5 than in RCP4.5 in response to elevated volcanic aerosols is due to a factor of 2.5 greater methane in RCP8.5 compared with RCP4.5. Our results demonstrate the substantial uncertainties in stratospheric ozone projections and expected recovery dates induced by volcanic aerosol perturbations that need to be considered in future model ozone projections.
Paulot, Fabien, David J Paynter, Paul Ginoux, Vaishali Naik, S Whitburn, M Van Damme, L Clarisse, P-F Coheur, and Larry W Horowitz, August 2017: Gas-aerosol partitioning of ammonia in biomass burning plumes: implications for the interpretation of spaceborne observations of ammonia and the radiative forcing of ammonium nitrate. Geophysical Research Letters, 44(15), DOI:10.1002/2017GL074215. Abstract
Satellite–derived enhancement ratios of NH3 relative to CO column burden ( math formula) in fires over Alaska, the Amazon, and South Equatorial Africa are 35, 45, and 70% lower than the corresponding ratio of their emissions factors ( math formula) from biomass burning derived from in-situ observations. Simulations performed using the GFDL AM3 global chemistry–climate model show that these regional differences may not entirely stem from an overestimate of NH3 emissions but rather from changes in the gas-aerosol partitioning of NH3 to NH math formula. Differences between math formula and math formula are largest in regions where EFNOx/NH3 is high, consistent with the production of NH4NO3. Biomass burning is estimated to contribute 13–24% of the global burden and direct radiative effect (DRE) of NH4NO3(-15 – -28 mWm−2), despite accounting for less than 6% of the global source of NH3. Production of NH4NO3 is largely concentrated over the Amazon and South Equatorial Africa, where its DRE can reach -1.9Wm−2 during the biomass burning season.
Saikawa, E, Hankyul Kim, M Zhong, Greet Janssens-Manehout, J Kurokawa, Zbigniew Klimont, F Wagner, Vaishali Naik, Larry W Horowitz, and Q Zhang, May 2017: Comparison of Emissions Inventories of Anthropogenic Air Pollutants in China. Atmospheric Chemistry and Physics Discussions, 17(10), DOI:10.5194/acp-17-6393-2017. Abstract
Anthropogenic air pollutant emissions have been increasing rapidly in China. Modelers use emissions inventories to assess temporal and spatial distribution of these emissions to estimate their impacts on regional and global air quality. However, large uncertainties exist in emissions estimates and assessing discrepancies in these inventories is essential for better understanding of the trends in air pollution over China. We compare five different emissions inventories estimating emissions of carbon monoxide (CO), nitrogen oxides (NOx), sulfur dioxide (SO2), particulate matter with an aerodynamic diameter of 10 um or less (PM10) from China. The emissions inventories analyzed in this paper include Regional Emissions inventory in ASia v2.1 (REAS); Multi-resolution Emission Inventory for China (MEIC); Emission Database for Global Atmospheric Research v4.2 (EDGAR); the inventory by Yu Zhao (ZHAO); and the Greenhouse Gas and Air Pollution Interactions and Synergies (GAINS). We focus on the period between 2000 and 2008 during which the Chinese economic activities have more than doubled. In addition to the national total, we also analyzed emissions from four source sectors (industry, transportation, power, and residential) and within seven regions in China (East, North, Northeast, Central, Southwest, Northwest, and South) and found that large disagreements (~ seven fold) exist among the five inventories at disaggregated levels. These discrepancies lead to differences of 67 ug/m3, 15 ppbv, and 470 ppbv for monthly mean PM10, O3, and CO, respectively, in modelled regional concentrations in China. We also find that MEIC inventory emissions estimates create a VOC-limited environment that produces much lower O3 mixing ratio in the East and Central China compared to the simulations using REAS and EDGAR estimates. Our results illustrate that a better understanding of Chinese emissions at more disaggregated levels is essential for finding an effective mitigation measure for reducing national and regional air pollution in China.
Saunois, Marielle, Philippe Bousquet, Ben Poulter, Philippe Ciais, Josep G Canadell, Edward J Dlugokencky, Giuseppe Etiope, David Bastviken, Sander Houweling, Greet Janssens-Manehout, F N Tubiello, Simona Castaldi, Robert B Jackson, M Alexe, Vivek Arora, D J Beerling, Peter Bergamaschi, Donald R Blake, Gordon Brailsford, Lori Bruhwiler, Cyril Crevoisier, Patrick Crill, C Covey, Christian Frankenberg, Nicola Gedney, Lena Höglund-Isaksson, Misa Ishizawa, Akihiko Ito, Fortunat Joos, Heon-Sook Kim, Thomas Kleinen, Paul Krummel, Jean-Francois Lamarque, Ray L Langenfelds, R Locatelli, Toshinobu Machida, Shamil Maksyutov, Joe R Melton, Isamu Morino, and Vaishali Naik, et al., September 2017: Variability and quasi-decadal changes in the methane budget over the period 2000–2012. Atmospheric Chemistry and Physics, 17(18), DOI:10.5194/acp-17-11135-2017. Abstract
Following the recent Global Carbon Project (GCP) synthesis of the decadal methane (CH4) budget over 2000–2012 (Saunois et al., 2016), we analyse here the same dataset with a focus on quasi-decadal and inter-annual variability in CH4 emissions. The GCP dataset integrates results from top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models (including process-based models for estimating land surface emissions and atmospheric chemistry), inventories of anthropogenic emissions, and data-driven approaches.
The annual global methane emissions from top-down studies, which by construction match the observed methane growth rate within their uncertainties, all show an increase in total methane emissions over the period 2000–2012, but this increase is not linear over the 13 years. Despite differences between individual studies, the mean emission anomaly of the top-down ensemble shows no significant trend in total methane emissions over the period 2000–2006, during the plateau of atmospheric methane mole fractions, and also over the period 2008–2012, during the renewed atmospheric methane increase. However, the top-down ensemble mean produces an emission shift between 2006 and 2008, leading to 22 [16–32] Tg CH4 yr−1 higher methane emissions over the period 2008–2012 compared to 2002–2006. This emission increase mostly originated from the tropics, with a smaller contribution from mid-latitudes and no significant change from boreal regions.
The regional contributions remain uncertain in top-down studies. Tropical South America and South and East Asia seem to contribute the most to the emission increase in the tropics. However, these two regions have only limited atmospheric measurements and remain therefore poorly constrained.
The sectorial partitioning of this emission increase between the periods 2002–2006 and 2008–2012 differs from one atmospheric inversion study to another. However, all top-down studies suggest smaller changes in fossil fuel emissions (from oil, gas, and coal industries) compared to the mean of the bottom-up inventories included in this study. This difference is partly driven by a smaller emission change in China from the top-down studies compared to the estimate in the Emission Database for Global Atmospheric Research (EDGARv4.2) inventory, which should be revised to smaller values in a near future. We apply isotopic signatures to the emission changes estimated for individual studies based on five emission sectors and find that for six individual top-down studies (out of eight) the average isotopic signature of the emission changes is not consistent with the observed change in atmospheric 13CH4. However, the partitioning in emission change derived from the ensemble mean is consistent with this isotopic constraint. At the global scale, the top-down ensemble mean suggests that the dominant contribution to the resumed atmospheric CH4 growth after 2006 comes from microbial sources (more from agriculture and waste sectors than from natural wetlands), with an uncertain but smaller contribution from fossil CH4 emissions. In addition, a decrease in biomass burning emissions (in agreement with the biomass burning emission databases) makes the balance of sources consistent with atmospheric 13CH4 observations.
In most of the top-down studies included here, OH concentrations are considered constant over the years (seasonal variations but without any inter-annual variability). As a result, the methane loss (in particular through OH oxidation) varies mainly through the change in methane concentrations and not its oxidants. For these reasons, changes in the methane loss could not be properly investigated in this study, although it may play a significant role in the recent atmospheric methane changes as briefly discussed at the end of the paper.
Silva, R A., J Jason West, Jean-Francois Lamarque, Drew Shindell, William J Collins, G Faluvegi, Gerd Folberth, Larry W Horowitz, T Nagashima, and Vaishali Naik, et al., September 2017: Future global mortality from changes in air pollution attributable to climate change. Nature Climate Change, 7(9), DOI:10.1038/nclimate3354. Abstract
Ground-level ozone and fine particulate matter (PM 2.5) are associated with premature human mortality1, 2, 3, 4; their future concentrations depend on changes in emissions, which dominate the near-term5, and on climate change6, 7. Previous global studies of the air-quality-related health effects of future climate change8, 9 used single atmospheric models. However, in related studies, mortality results differ among models10, 11, 12. Here we use an ensemble of global chemistry–climate models13 to show that premature mortality from changes in air pollution attributable to climate change, under the high greenhouse gas scenario RCP8.5 (ref. 14), is probably positive. We estimate 3,340 (−30,300 to 47,100) ozone-related deaths in 2030, relative to 2000 climate, and 43,600 (−195,000 to 237,000) in 2100 (14% of the increase in global ozone-related mortality). For PM 2.5, we estimate 55,600 (−34,300 to 164,000) deaths in 2030 and 215,000 (−76,100 to 595,000) in 2100 (countering by 16% the global decrease in PM 2.5-related mortality). Premature mortality attributable to climate change is estimated to be positive in all regions except Africa, and is greatest in India and East Asia. Most individual models yield increased mortality from climate change, but some yield decreases, suggesting caution in interpreting results from a single model. Climate change mitigation is likely to reduce air-pollution-related mortality.
West, J J., Y Zhang, Steven J Smith, R A Silva, J H Bowden, Vaishali Naik, Y Li, D Gilfillan, Z Adelman, M Fry, S C Anenberg, Larry W Horowitz, and Jean-Francois Lamarque, April 2017: Cobenefits of global and domestic greenhouse gas emissions for air quality and human health. The Lancet, 389(S23), DOI:10.1016/S0140-6736(17)31135-2.
Parrish, David D., Ian E Galbally, Jean-Francois Lamarque, Vaishali Naik, and Larry W Horowitz, et al., January 2016: Seasonal cycles of O3 in the marine boundary layer: Observation and model simulation comparisons. Journal of Geophysical Research: Atmospheres, 121(1), DOI:10.1002/2015JD024101. Abstract
We present a two-step approach for quantitatively comparing modeled and measured seasonal cycles of O3: 1) fitting sine functions to monthly averaged measurements and model results (i.e. deriving a Fourier series expansion of these results), and 2) comparing the phase and amplitude of the statistically significant terms between the models and measurements. Two and only two sine terms are sufficient to quantify the O3 seasonal cycle in the marine boundary layer (MBL) in both the measurements and the model results. In addition to the expected fundamental (one sine cycle per year), a 2nd harmonic term (i.e. two sine cycles per year) is identified as a ubiquitous feature of O3 in the MBL. Three chemistry climate models (CAM-chem, GFDL-CM3 and GISS-E2-R) approximately reproduce many features of the measured seasonal cycles at MBL surface sites throughout the globe, with some notable quantitative disagreements, but give divergent results that do not agree with O3 sonde measurements above the MBL. This disagreement and divergence of results between models indicate that the treatment of the MBL dynamics in the CCMs is not adequate to reproduce the isolation of the MBL indicated by the observations. Within the MBL the models more accurately reproduce the second harmonic term than the fundamental term. We attribute the second harmonic term to the second harmonic of opposite phase in the photolysis rate of O3, while the fundamental term evidently has many influences. The parameters derived from the Fourier series expansion of the measurements are quantitative metrics that can serve as the basis for future model-measurement comparisons.
We update and evaluate the treatment of nitrate aerosols in the Geophysical Fluid Dynamics Laboratory (GFDL) atmospheric model (AM3). Accounting for the radiative effects of nitrate aerosols generally improves the simulated aerosol optical depth, although nitrate concentrations at the surface are biased high. This bias can be reduced by increasing the deposition of nitrate to account for the near-surface volatilization of ammonium nitrate or by neglecting the heterogeneous production of nitric acid to account for the inhibition of N2O5 reactive uptake at high nitrate concentrations. Globally, uncertainties in these processes can impact the simulated nitrate optical depth by up to 25 %, much more than the impact of uncertainties in the seasonality of ammonia emissions (6 %) or in the uptake of nitric acid on dust (13 %). Our best estimate for present-day fine nitrate optical depth at 550 nm is 0.006 (0.005–0.008). We only find a modest increase of nitrate optical depth (< 30 %) in response to the projected changes in the emissions of SO2 (−40 %) and ammonia (+38 %) from 2010 to 2050. Nitrate burden is projected to increase in the tropics and in the free troposphere, but to decrease at the surface in the midlatitudes because of lower nitric acid concentrations. Our results suggest that better constraints on the heterogeneous chemistry of nitric acid on dust, on tropical ammonia emissions, and on the transport of ammonia to the free troposphere are needed to improve projections of aerosol optical depth.
Saunois, Marielle, Philippe Bousquet, Ben Poulter, A Peregon, Philippe Ciais, Josep G Canadell, Edward J Dlugokencky, Giuseppe Etiope, David Bastviken, Sander Houweling, Greet Janssens-Manehout, F N Tubiello, Simona Castaldi, Robert B Jackson, M Alexe, Vivek Arora, D J Beerling, Peter Bergamaschi, Donald R Blake, Gordon Brailsford, Victor Brovkin, Lori Bruhwiler, Cyril Crevoisier, Patrick Crill, C Covey, Charles Curry, Christian Frankenberg, Nicola Gedney, Lena Höglund-Isaksson, Misa Ishizawa, Akihiko Ito, Fortunat Joos, Heon-Sook Kim, Thomas Kleinen, Paul Krummel, Jean-Francois Lamarque, Ray L Langenfelds, R Locatelli, Toshinobu Machida, Shamil Maksyutov, Kyle C McDonald, J Marshall, Joe R Melton, Isamu Morino, and Vaishali Naik, et al., December 2016: The global methane budget 2000–2012. Earth System Science Data, 8(2), DOI:10.5194/essd-8-697-2016. Abstract
The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase, making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (∼ biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations).
For the 2003–2012 decade, global methane emissions are estimated by top-down inversions at 558 Tg CH4 yr−1, range 540–568. About 60 % of global emissions are anthropogenic (range 50–65 %). Since 2010, the bottom-up global emission inventories have been closer to methane emissions in the most carbon-intensive Representative Concentrations Pathway (RCP8.5) and higher than all other RCP scenarios. Bottom-up approaches suggest larger global emissions (736 Tg CH4 yr−1, range 596–884) mostly because of larger natural emissions from individual sources such as inland waters, natural wetlands and geological sources. Considering the atmospheric constraints on the top-down budget, it is likely that some of the individual emissions reported by the bottom-up approaches are overestimated, leading to too large global emissions. Latitudinal data from top-down emissions indicate a predominance of tropical emissions (∼ 64 % of the global budget, < 30° N) as compared to mid (∼ 32 %, 30–60° N) and high northern latitudes (∼ 4 %, 60–90° N). Top-down inversions consistently infer lower emissions in China (∼ 58 Tg CH4 yr−1, range 51–72, −14 %) and higher emissions in Africa (86 Tg CH4 yr−1, range 73–108, +19 %) than bottom-up values used as prior estimates. Overall, uncertainties for anthropogenic emissions appear smaller than those from natural sources, and the uncertainties on source categories appear larger for top-down inversions than for bottom-up inventories and models.
The most important source of uncertainty on the methane budget is attributable to emissions from wetland and other inland waters. We show that the wetland extent could contribute 30–40 % on the estimated range for wetland emissions. Other priorities for improving the methane budget include the following: (i) the development of process-based models for inland-water emissions, (ii) the intensification of methane observations at local scale (flux measurements) to constrain bottom-up land surface models, and at regional scale (surface networks and satellites) to constrain top-down inversions, (iii) improvements in the estimation of atmospheric loss by OH, and (iv) improvements of the transport models integrated in top-down inversions. The data presented here can be downloaded from the Carbon Dioxide Information Analysis Center (http://doi.org/10.3334/CDIAC/GLOBAL_METHANE_BUDGET_2016_V1.1) and the Global Carbon Project.
The effect of future climate change on surface ozone over North America, Europe, and East Asia is evaluated using present-day (2000s) and future (2100s) hourly surface ozone simulated by four global models. Future climate follows RCP8.5, while methane and anthropogenic ozone precursors are fixed at year-2000 levels. Climate change shifts the seasonal surface ozone peak to earlier in the year and increases the amplitude of the annual cycle. Increases in mean summertime and high-percentile ozone are generally found in polluted environments, while decreases are found in clean environments. We propose climate change augments the efficiency of precursor emissions to generate surface ozone in polluted regions, thus reducing precursor export to neighboring downwind locations. Even with constant biogenic emissions, climate change causes the largest ozone increases at high percentiles. In most cases, air quality extreme episodes become larger and contain higher ozone levels relative to the rest of the distribution.
Silva, R A., J Jason West, Jean-Francois Lamarque, Drew Shindell, William J Collins, S Dalsoren, G Faluvegi, Gerd Folberth, Larry W Horowitz, T Nagashima, and Vaishali Naik, et al., August 2016: The effect of future ambient air pollution on human premature mortality to 2100 using output from the ACCMIP model ensemble. Atmospheric Chemistry and Physics, 16(15), DOI:10.5194/acp-16-9847-2016. Abstract
Ambient air pollution from ground-level ozone and fine particulate matter (PM2.5) is associated with premature mortality. Future concentrations of these air pollutants will be driven by natural and anthropogenic emissions and by climate change. Using anthropogenic and biomass burning emissions projected in the four Representative Concentration Pathway scenarios (RCPs), the ACCMIP ensemble of chemistry-climate models simulated future concentrations of ozone and PM2.5 at selected decades between 2000 and 2100. We use output from the ACCMIP ensemble, together with projections of future population and baseline mortality rates, to quantify the human premature mortality impacts of future ambient air pollution. Future air pollution-related premature mortality in 2030, 2050 and 2100 is estimated for each scenario and for each model using a health impact function based on changes in concentrations of ozone and PM2.5 relative to 2000 and projected future population and baseline mortality rates. Additionally, the global mortality burden of ozone and PM2.5 in 2000 and each future period is estimated relative to 1850 concentrations, using present-day and future population and baseline mortality rates. The change in future ozone concentrations relative to 2000 is associated with excess global premature mortality in some scenarios/periods, particularly in RCP8.5 in 2100 (316 thousand deaths/year), likely driven by the large increase in methane emissions and by the net effect of climate change projected in this scenario, but it leads to considerable avoided premature mortality for the three other RCPs. However, the global mortality burden of ozone markedly increases from less than 0.4 million deaths/year in 2000 to between 1.09 and 2.36 million deaths/year in 2100, across RCPs, mostly due to the effect of increases in population and baseline mortality rates. Decreases in PM2.5 concentrations relative to 2000 are associated with avoided premature mortality in all scenarios, particularly in 2100: between −2.39 and −1.31 million deaths/year for the four RCPs due to the reductions in emissions projected in these scenarios. The global mortality burden of PM2.5 is estimated to decrease from 1.7 million deaths/year in 2000 to between 0.95 and 1.55 million deaths/year in 2100 for the four RCPs, due to the combined effect of decreases in PM2.5 concentrations and changes in population and baseline mortality rates. Trends in future air pollution-related mortality vary regionally across scenarios, reflecting assumptions for economic growth and air pollution control specific to each RCP and region. Mortality estimates differ among chemistry-climate models due to differences in simulated pollutant concentrations, and is the greatest contributor to overall mortality uncertainty for most cases assessed here, supporting the use of model ensembles to characterize uncertainty. Increases in exposed population and baseline mortality rates of respiratory diseases magnify the impact on premature mortality of changes in future air pollutant concentrations and explain why the future global mortality burden of air pollution can exceed the current burden, even where air pollutant concentrations decrease.
Climate change can influence fine particulate matter concentrations (PM2.5) through changes in air pollution meteorology. Knowledge of the extent to which climate change can exacerbate or alleviate air pollution in the future is needed for robust climate and air pollution policy decision-making. To examine the influence of climate on PM2.5, we use the Geophysical Fluid Dynamics Laboratory Coupled Model version 3 (GFDL CM3), a fully-coupled chemistry-climate model, combined with future emissions and concentrations provided by the four Representative Concentration Pathways (RCPs). For each of the RCPs, we conduct future simulations in which emissions of aerosols and their precursors are held at 2005 levels while other climate forcing agents evolve in time, such that only climate (and thus meteorology) can influence PM2.5 surface concentrations. We find a small increase in global, annual mean PM2.5 of about 0.21 μg m−3 (5%) for RCP8.5, a scenario with maximum warming. Changes in global mean PM2.5 are at a maximum in the fall and are mainly controlled by sulfate followed by organic aerosol with minimal influence of black carbon. RCP2.6 is the only scenario that projects a decrease in global PM2.5 with future climate changes, albeit only by −0.06 μg m−3 (1.5%) by the end of the 21st century. Regional and local changes in PM2.5 are larger, reaching upwards of 2 μg m−3 for polluted (eastern China) and dusty (western Africa) locations on an annually averaged basis in RCP8.5. Using multiple linear regression, we find that future PM2.5 concentrations are most sensitive to local temperature, followed by surface wind and precipitation. PM2.5 concentrations are robustly positively associated with temperature, while negatively related with precipitation and wind speed. Present-day (2006–2015) modeled sensitivities of PM2.5 to meteorological variables are evaluated against observations and found to agree reasonably well with observed sensitivities (within 10–50% over the eastern United States for several variables), although the modeled PM2.5 is less sensitive to precipitation than in the observations due to weaker convective scavenging. We conclude that the hypothesized “climate penalty” of future increases in PM2.5 is relatively minor on a global scale compared to the influence of emissions on PM2.5 concentrations.
Zhang, Y, J H Bowden, Z Adelman, Vaishali Naik, Larry W Horowitz, Steven J Smith, and J Jason West, August 2016: Co-benefits of global and regional greenhouse gas mitigation on U.S. air quality in 2050. Atmospheric Chemistry and Physics, 16(15), DOI:10.5194/acp-16-9533-2016. Abstract
Policies to mitigate greenhouse gas (GHG) emissions will not only slow climate change, but can also have ancillary benefits of improved air quality. Here we examine the co-benefits of both global and regional GHG mitigation on U.S. air quality in 2050 at fine resolution, using dynamical downscaling methods, building on a previous global co-benefits study (West et al., 2013). The co-benefits for U.S. air quality are quantified via two mechanisms: through reductions in co-emitted air pollutants from the same sources, and by slowing climate change and its influence on air quality, following West et al. (2013). Additionally, we separate the total co-benefits into contributions from domestic GHG mitigation versus mitigation in foreign countries. We use the WRF model to dynamically downscale future global climate to the regional scale, the SMOKE program to directly process global anthropogenic emissions into the regional domain, and we provide dynamical boundary conditions from global simulations to the regional CMAQ model. The total co-benefits of global GHG mitigation from the RCP4.5 scenario compared with its reference are estimated to be higher in the eastern U.S. (ranging from 0.6–1.0 μg m-3) than the west (0–0.4 μg m-3) for PM2.5, with an average of 0.47 μg m-3 over U.S.; for O3, the total co-benefits are more uniform at 2–5 ppb with U.S. average of 3.55 ppb. Comparing the two mechanisms of co-benefits, we find that reductions of co-emitted air pollutants have a much greater influence on both PM2.5 (96 % of the total co-benefits) and O3 (89 % of the total) than the second co-benefits mechanism via slowing climate change, consistent with West et al. (2013). GHG mitigation from foreign countries contributes more to the U.S. O3 reduction (76 % of the total) than that from domestic GHG mitigation only (24 %), highlighting the importance of global methane reductions and the intercontinental transport of air pollutants. For PM2.5, the benefits of domestic GHG control are greater (74 % of total). Since foreign contributions to the co-benefits are comparable to that from the domestic reductions, especially for O3, previous studies that focus on local or regional co-benefits may greatly underestimate the total co-benefits of global GHG reductions. We conclude that the U.S. can gain significantly greater domestic air quality co-benefits by engaging with other nations to control GHGs.
Zhong, M, E Saikawa, Y Liu, Vaishali Naik, and Larry W Horowitz, et al., April 2016: Air Quality Modeling with WRF-Chem v3.5 in East and South Asia: sensitivity to emissions and evaluation of simulated air quality. Geoscientific Model Development, 9(3), DOI:10.5194/gmd-9-1201-2016. Abstract
We conducted simulations using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) version 3.5 to study air quality in East and South Asia at a spatial resolution of 20 km × 20 km. We find large discrepancies between two existing emissions inventories: the Regional Emission Inventory in Asia version 2 (REAS) and the Emissions Database for Global Atmospheric Research version 4.2 (EDGAR) at the provincial level in China, with maximum differences up to 500 % for CO emissions, 190 % for NO, and 160 % for primary PM10. Such differences in the magnitude and the spatial distribution of emissions for various species lead to 40–70 % difference in surface PM10 concentrations, 16–20 % in surface O3 mixing ratios, and over 100 % in SO2 and NO2 mixing ratios in the polluted areas of China. Our sensitivity run shows WRF-Chem is sensitive to emissions, with the REAS-based simulation reproducing observed concentrations and mixing ratios better than the EDGAR-based simulation for July 2007. We conduct further model simulations using REAS emissions for January, April, July, and October in 2007 and evaluate simulations with available ground-level observations. The model results show clear regional variations in the seasonal cycle of surface PM10 and O3 over East and South Asia. The model meets the air quality model performance criteria for both PM10 (mean fractional bias, MFB ≤ ± 60 %) and O3 (MFB ≤ ± 15 %) in most of the observation sites, although the model underestimates PM10 over Northeast China in January. The model predicts the observed SO2 well at sites in Japan, while it tends to overestimate SO2 in China in July and October. The model underestimates most observed NO2 in all four months. These findings suggest that future model development and evaluation of emission inventories and models are needed for particulate matter and gaseous pollutants in East and South Asia.
Multiple linkages connect air quality and climate change. Many air pollutant sources also emit carbon dioxide (CO2), the dominant anthropogenic greenhouse gas (GHG). The two main contributors to non-attainment of U.S. ambient air quality standards, ozone (O3) and particulate matter (PM), interact with radiation, forcing climate change. PM warms by absorbing sunlight (e.g., black carbon) or cools by scattering sunlight (e.g., sulfates) and interacts with clouds; these radiative and microphysical interactions can induce changes in precipitation and regional circulation patterns. Climate change is expected to degrade air quality in many polluted regions by changing air pollution meteorology (ventilation and dilution), precipitation and other removal processes, and by triggering some amplifying responses in atmospheric chemistry and in anthropogenic and natural sources. Together, these processes shape distributions and extreme episodes of O3 and PM. Global modeling indicates that as air pollution programs reduce SO2 to meet health and other air quality goals, near-term warming accelerates due to “unmasking” of warming induced by rising CO2. Air pollutant controls on CH4, a potent GHG and precursor to global O3 levels, and on sources with high black carbon (BC) to organic carbon (OC) ratios could offset near-term warming induced by SO2 emission reductions, while reducing global background O3 and regionally high levels of PM. Lowering peak warming requires decreasing atmospheric CO2, which for some source categories would also reduce co-emitted air pollutants or their precursors. Model projections for alternative climate and air quality scenarios indicate a wide range for U.S. surface O3 and fine PM, although regional projections may be confounded by interannual to decadal natural climate variability. Continued implementation of U.S. NOx emission controls guards against rising pollution levels triggered either by climate change or by global emission growth. Improved accuracy and trends in emission inventories are critical for accountability analyses of historical and projected air pollution and climate mitigation policies.
Rieder, H E., Arlene M Fiore, Larry W Horowitz, and Vaishali Naik, January 2015: Projecting policy-relevant metrics for high summertime ozone pollution events over the eastern United States due to climate and emission changes during the 21st century. Journal of Geophysical Research: Atmospheres, 120(2), DOI:10.1002/2014JD022303. Abstract
Over the eastern United States (EUS), nitrogen oxides (NOx) emission controls have led to improved air quality over the past two decades, but concerns have been raised that climate warming may offset some of these gains. Here we analyze the effect of changing emissions and climate, in isolation and combination, on EUS summertime surface ozone (O3) over the recent past and the 21st century in an ensemble of simulations performed with the Geophysical Fluid Dynamics Laboratory CM3 chemistry-climate model. The simulated summertime EUS O3 is biased high but captures the structure of observed changes in regional O3 distributions following NOx emission reductions. We introduce a statistical bias correction, which allows derivation of policy-relevant statistics by assuming a stationary mean state bias in the model, but accurate simulation of changes at each quantile of the distribution. We contrast two different 21st century scenarios: (i) representative concentration pathway (RCP) 4.5 and (ii) simulations with well-mixed greenhouse gases (WMGG) following RCP4.5 but with emissions of air pollutants and precursors held fixed at 2005 levels (RCP4.5_WMGG). We find under RCP4.5 no exceedance of maximum daily 8 hour average ozone above 75 ppb by mid-21st century, reflecting the U.S. NOx emissions reductions projected in RCP4.5, while more than half of the EUS exceeds this level by the end of the 21st century under RCP4.5_WMGG. Further, we find a simple relationship between the changes in estimated 1 year return levels and regional NOx emission changes, implying that our results can be generalized to estimate changes in the frequency of EUS pollution events under different regional NOx emission scenarios.
We test the current generation of global chemistry-climate models in their ability to simulate observed, present-day surface ozone. Models are evaluated against hourly surface ozone from 4217 stations in North America and Europe that are averaged over 1° × 1° grid cells, allowing commensurate model-measurement comparison. Models are generally biased high during all hours of the day and in all regions. Most models simulate the shape of regional summertime diurnal and annual cycles well, correctly matching the timing of hourly (~ 15:00) and monthly (mid-June) peak surface ozone abundance. The amplitude of these cycles is less successfully matched. The observed summertime diurnal range (~ 25 ppb) is underestimated in all regions by about 7 ppb, and the observed seasonal range (~ 21 ppb) is underestimated by about 5 ppb except in the most polluted regions where it is overestimated by about 5 ppb. The models generally match the pattern of the observed summertime ozone enhancement, but they overestimate its magnitude in most regions. Most models capture the observed distribution of extreme episode sizes, correctly showing that about 80% of individual extreme events occur in large-scale, multi-day episodes of more than 100 grid cells. The observed linear relationship showing increases in ozone by up to 6 ppb for larger-sized episodes is also matched.
Westervelt, Daniel M., Larry W Horowitz, Vaishali Naik, and D L Mauzerall, November 2015: Radiative forcing and climate response to projected 21st century aerosol decreases. Atmospheric Chemistry and Physics, 15(22), DOI:10.5194/acp-15-12681-2015. Abstract
It is widely expected that global emissions of atmospheric aerosols and their precursors will decrease strongly throughout the remainder of the 21st century, due to emission reduction policies enacted to protect human health. For instance, global emissions of aerosols and their precursors are projected to decrease by as much as 80% by the year 2100, according to the four Representative Concentration Pathway (RCP) scenarios. The removal of aerosols will cause unintended climate consequences, including an unmasking of global warming from long-lived greenhouse gases. We use the Geophysical Fluid Dynamics Laboratory Climate Model version 3 (GFDL CM3) to simulate future climate over the 21st century with and without the aerosol emission changes projected by each of the RCPs in order to isolate the radiative forcing and climate response resulting from the aerosol reductions. We find that the projected global radiative forcing and climate response due to aerosol decreases do not vary significantly across the four RCPs by 2100, although there is some mid-century variation, especially in cloud droplet effective radius, that closely follows the RCP emissions and energy consumption projections. Up to 1 W m−2 of radiative forcing may be unmasked globally from 2005 to 2100 due to reductions in aerosol and precursor emissions, leading to average global temperature increases up to 1 K and global precipitation rate increases up to 0.09 mm d−1. Regionally and locally, climate impacts can be much larger, with a 2.1 K warming projected over China, Japan, and Korea due to the reduced aerosol emissions in RCP8.5, as well as nearly a 0.2 mm d−1 precipitation increase, a 7 g m−2 LWP decrease, and a 2 μm increase in cloud droplet effective radius. Future aerosol decreases could be responsible for 30–40% of total climate warming by 2100 in East Asia, even under the high greenhouse gas emissions scenario (RCP8.5). The expected unmasking of global warming caused by aerosol reductions will require more aggressive greenhouse gas mitigation policies than anticipated in order to meet desired climate targets.
The late 20th century response of the South Asian monsoon to changes in anthropogenic aerosols from local (i.e., South Asia) and remote (i.e., outside South Asia) sources was investigated using historical simulations with a state-of-the-art climate model. The observed summertime drying over India is replaced by widespread wettening once local aerosol emissions are kept at pre-industrial levels while all the other forcings evolve. Constant remote aerosol emissions partially suppress the precipitation decrease. While predominant precipitation changes over India are thus associated with local aerosols, remote aerosols contribute as well, especially in favoring an earlier monsoon onset in June and enhancing summertime rainfall over the northwestern regions. Conversely, temperature and near-surface circulation changes over South Asia are more effectively driven by remote aerosols. These changes are reflected into northward cross-equatorial anomalies in the atmospheric energy transport induced by both local and, to a greater extent, remote aerosols.
Changing emissions can alter the surface O3 seasonal cycle, as detected from Northeastern U.S. (NE) observations during recent decades. Under continued regional precursor emission controls (-72% NE NOx by 2100), the NE surface O3 seasonal cycle reverses (to a winter maximum) in 21st Century transient chemistry-climate simulations. Over polluted regions, regional NOx largely controls the shape of surface O3 seasonal cycles. In the absence of regional NOx controls, climate warming contributes to a higher surface O3 summertime peak over the NE. A doubling of the global CH4 abundance by 2100 partially offsets summertime surface O3 decreases attained via NOx reductions and contributes to raising surface O3 during December-March when the O3 lifetime is longer. The similarity between surface O3 seasonal cycles over the NE and the InterMountain West by 2100 indicates a NE transition to a region representative of baseline surface O3 conditions.
Cooper, Owen R., David D Parrish, J R Ziemke, N V Balashov, M Cupeiro, Ian E Galbally, S Gilge, Larry W Horowitz, N R Jensen, Jean-Francois Lamarque, and Vaishali Naik, et al., July 2014: Global distribution and trends of tropospheric ozone: An observation-based review. Elementa: Science of the Anthropocene, 2, 000029, DOI:10.12952/journal.elementa.000029. Abstract
Tropospheric ozone plays a major role in Earth’s atmospheric chemistry processes and also acts as an air pollutant and greenhouse gas. Due to its short lifetime, and dependence on sunlight and precursor emissions from natural and anthropogenic sources, tropospheric ozone’s abundance is highly variable in space and time on seasonal, interannual and decadal time-scales. Recent, and sometimes rapid, changes in observed ozone mixing ratios and ozone precursor emissions inspired us to produce this up-to-date overview of tropospheric ozone’s global distribution and trends. Much of the text is a synthesis of in situ and remotely sensed ozone observations reported in the peer-reviewed literature, but we also include some new and extended analyses using well-known and referenced datasets to draw connections between ozone trends and distributions in different regions of the world. In addition, we provide a brief evaluation of the accuracy of rural or remote surface ozone trends calculated by three state-of-the-science chemistry-climate models, the tools used by scientists to fill the gaps in our knowledge of global tropospheric ozone distribution and trends.
Accurate estimates for North American background (NAB) ozone (O3) in surface air over the United States are needed for setting and implementing an attainable national O3 standard. These estimates rely on simulations with atmospheric chemistry-transport models that set North American anthropogenic emissions to zero, and to date have relied heavily on one global model. We examine NAB estimates for spring and summer 2006 with two independent global models (GEOS-Chem and GFDL AM3). We evaluate the base simulations, which include North American anthropogenic emissions, with mid-tropospheric O3 retrieved from space and ground-level O3 measurements. The models often bracket the observed values, implying value in developing a multi-model approach to estimate NAB O3. Consistent with earlier studies, the models robustly simulate the largest nation-wide NAB levels at high-altitude western U.S. sites (seasonal average maximum daily 8-h values of ∼40–50 ppb in spring and ∼25–40 ppb in summer) where it correlates with observed O3. At these sites, a 27-year GFDL AM3 simulation simulates observed O3 events above 60 ppb and indicates that year-to-year variations in NAB O3 influence their annual frequency (with NAB contributing 50–60 ppb or more during individual events). During summer over the eastern United States (EUS), when photochemical production from regional anthropogenic emissions peaks, NAB is largely uncorrelated with observed values and it is lower than at high-altitude sites (average values of ∼20–30 ppb). Four processes contribute substantially to model differences in specific regions and seasons: lightning NOx, biogenic isoprene emissions and chemistry, wildfires, and stratosphere-to-troposphere transport. Differences in the representations of these processes within the GFDL AM3 and GEOS-Chem models contribute more to uncertainty in NAB estimates, particularly in spring when NAB is highest, than the choice of horizontal resolution within a single model (GEOS-Chem). We propose that future efforts seek to constrain these processes with targeted analysis of multi-model simulations evaluated with observations of O3 and related species from multiple platforms, and thereby reduce the error on NAB estimates needed for air quality planning.
Parrish, David D., Jean-Francois Lamarque, Vaishali Naik, and Larry W Horowitz, et al., May 2014: Long-term changes in lower tropospheric baseline ozone concentrations: Comparing chemistry-climate models and observations at northern mid-latitudes. Journal of Geophysical Research: Atmospheres, 119(9), DOI:10.1002/2013JD021435. Abstract
Two recent papers have quantified long-term ozone (O3) changes observed at northern mid-latitude sites that are believed to represent baseline (here understood as representative of continental to hemispheric scales) conditions. Three chemistry climate models (NCAR CAM-chem, GFDL-CM3 and GISS-E2-R) have calculated retrospective tropospheric O3 concentrations as part of the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) and Coupled Model Intercomparison Project Phase 5 (CMIP5) model intercomparisons. We present an approach for quantitative comparisons of model results with measurements for seasonally averaged O3 concentrations. There is considerable qualitative agreement between the measurements and the models, but there are also substantial and consistent quantitative disagreements. Most notably models 1) overestimate absolute O3 mixing ratios, on average by ~5 to 17 ppbv in the year 2000, 2) capture only ~50% of O3 changes observed over the past five to six decades, and little of observed seasonal differences, and 3) capture ~25 to 45% of the rate of change of the long-term changes. These disagreements are significant enough to indicate that only limited confidence can be placed on estimates of present-day radiative forcing of tropospheric O3 derived from modeled historic concentration changes and on predicted future O3 concentrations. Evidently our understanding of tropospheric O3, or the incorporation of chemistry and transport processes into current chemical climate models, is incomplete. Modeled O3 trends approximately parallel estimated trends in anthropogenic emissions of NOX, an important O3 precursor, while measured O3 changes increase more rapidly than these emission estimates.
Bowman, K W., Larry W Horowitz, and Vaishali Naik, April 2013: Evaluation of ACCMIP outgoing longwave radiation from tropospheric ozone using TES satellite observations. Atmospheric Chemistry and Physics, 13(8), DOI:10.5194/acp-13-4057-2013. Abstract
We use simultaneous observations of tropospheric ozone and outgoing longwave radiation (OLR) sensitivity to tropospheric ozone from the Tropospheric Emission Spectrometer (TES) to evaluate model tropospheric ozone and its effect on OLR simulated by a suite of chemistry-climate models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean of ACCMIP models show a persistent but modest tropospheric ozone low bias (5–20 ppb) in the Southern Hemisphere (SH) and modest high bias (5–10 ppb) in the Northern Hemisphere (NH) relative to TES ozone for 2005–2010. These ozone biases have a significant impact on the OLR. Using TES instantaneous radiative kernels (IRK), we show that the ACCMIP ensemble mean tropospheric ozone low bias leads up to 120 mW m−2 OLR high bias locally but zonally compensating errors reduce the global OLR high bias to 39 ± 41 m Wm−2 relative to TES data. We show that there is a correlation (R2 = 0.59) between the magnitude of the ACCMIP OLR bias and the deviation of the ACCMIP preindustrial to present day (1750–2010) ozone radiative forcing (RF) from the ensemble ozone RF mean. However, this correlation is driven primarily by models whose absolute OLR bias from tropospheric ozone exceeds 100 m Wm−2. Removing these models leads to a mean ozone radiative forcing of 394 ± 42 m Wm−2. The mean is about the same and the standard deviation is about 30% lower than an ensemble ozone RF of 384 ± 60 m Wm−2 derived from 14 of the 16 ACCMIP models reported in a companion ACCMIP study. These results point towards a profitable direction of combining satellite observations and chemistry-climate model simulations to reduce uncertainty in ozone radiative forcing.
Fang, Y, Vaishali Naik, Larry W Horowitz, and D L Mauzerall, February 2013: Air pollution and associated human mortality: the role of air pollutant emissions, climate change and methane concentration increases from the preindustrial period to present. Atmospheric Chemistry and Physics, 13(3), DOI:10.5194/acp-13-1377-2013. Abstract
Increases in surface ozone (O3) and fine particulate matter (≤2.5 μm} aerodynamic diameter, PM2.5) are associated with excess premature human mortalities. Here we estimate changes in surface O3 and PM2.5 since preindustrial (1860) times and the global present-day (2000) premature human mortalities associated with these changes. We go beyond previous work to analyze and differentiate the contribution of three factors: changes in emissions of short-lived air pollutants, climate change, and increased methane (CH4) concentrations, to air pollution levels and the associated premature mortalities. We use a coupled chemistry-climate model in conjunction with global population distributions in 2000 to estimate exposure attributable to concentration changes since 1860 from each factor. Attributable mortalities are estimated using health impact functions of long-term relative risk estimates for O3 and PM2.5 from the epidemiology literature. We find global mean surface PM2.5 and health-relevant O3 (defined as the maximum 6-month mean of 1-h daily maximum O3 in a year) have increased by 8 ± 0.16 μg m−3 and 30 ± 0.16 ppbv, respectively, over this industrial period as a result of combined changes in emissions of air pollutants (EMIS), climate (CLIM) and CH4 concentrations (TCH4). EMIS, CLIM and TCH4 cause global average PM2.5(O3) to change by +7.5 ± 0.19 μg m−3 (+25 ± 0.30 ppbv), +0.4 ± 0.17 μg m−3 (+0.5 ± 0.28 ppbv), and −0.02 ± 0.01 μg m−3 (+4.3 ± 0.33 ppbv), respectively. Total changes in PM2.5 are associated with 1.5 (95% confidence interval, CI, 1.0–2.5) million all-cause mortalities annually and in O3 are associated with 375 (95% CI, 129–592) thousand respiratory mortalities annually. Most air pollution mortality is driven by changes in emissions of short-lived air pollutants and their precursors (95% and 85% of mortalities from PM2.5 and O3, respectively). However, changing climate and increasing CH4 concentrations also increased premature mortality associated with air pollution globally up to 5% and 15%, respectively. In some regions, the contribution of climate change and increased CH4 together are responsible for more than 20% of the respiratory mortality associated with O3 exposure. We find the interaction between climate change and atmospheric chemistry has influenced atmospheric composition and human mortality associated with industrial air pollution. In addition to driving 13% of the total historical changes in surface O3 and 15% of the associated mortalities, CH4 is the dominant factor driving changes in atmospheric OH and H2O2 since preindustrial time. Our study highlights the benefits to air quality and human health of CH4 mitigation as a component of future air pollution control policy.
Carbon monoxide (CO) emissions influence global and regional air quality and global climate change by affecting atmospheric oxidants and secondary species. We simulate the influence of halving anthropogenic CO emissions globally and individually from 10 regions on surface and tropospheric ozone, methane, and aerosol concentrations using a global chemical transport model (MOZART-4 for the year 2005). Net radiative forcing (RF) is then estimated using the GFDL standalone radiative transfer model. We estimate that halving global CO emissions decreases global annual average concentrations of surface ozone by 0.45 ppbv, tropospheric methane by 73 ppbv, and global annual net RF by 36.1 mW m−2, nearly equal to the sum of changes from the 10 regional reductions. Global annual net RF per unit change in emissions and the 100-yr global warming potential (GWP100) are estimated as −0.124 mW m−2 (Tg CO yr−1)−1 and 1.34, respectively, for the global CO reduction, and ranging from −0.115 to −0.131 mW m−2 (Tg CO yr−1)−1 and 1.26 to 1.44 across 10 regions, with the greatest sensitivities for regions in the tropics. The net RF distributions show widespread cooling corresponding to the O3 and CH4 decreases, and localized positive and negative net RFs due to changes in aerosols. The strongest annual net RF impacts occur within the tropics (28° S–28° N) followed by the northern mid-latitudes (28° N–60° N), independent of reduction region, while the greatest changes in surface CO and ozone concentrations occur within the reduction region. Some regional reductions strongly influence the air quality in other regions, such as East Asia, which has an impact on US surface ozone that is 93% of that from North America. Changes in the transport of CO and downwind ozone production clearly exceed the direct export of ozone from each reduction region. The small variation in CO GWPs among world regions suggests that future international climate agreements could adopt a globally uniform metric for CO with little error, or could use different GWPs for each continent. Doing so may increase the incentive to reduce CO through coordinated policies addressing climate and air quality.
Kirschke, S, and Vaishali Naik, et al., October 2013: Three decades of global methane sources and sinks. Nature Geoscience, 6(10), DOI:10.1038/ngeo1955. Abstract
Methane is an important greenhouse gas, responsible for about 20% of the warming induced by long-lived greenhouse gases since pre-industrial times. By reacting with hydroxyl radicals, methane reduces the oxidizing capacity of the atmosphere and generates ozone in the troposphere. Although most sources and sinks of methane have been identified, their relative contributions to atmospheric methane levels are highly uncertain. As such, the factors responsible for the observed stabilization of atmospheric methane levels in the early 2000s, and the renewed rise after 2006, remain unclear. Here, we construct decadal budgets for methane sources and sinks between 1980 and 2010, using a combination of atmospheric measurements and results from chemical transport models, ecosystem models, climate chemistry models and inventories of anthropogenic emissions. The resultant budgets suggest that data-driven approaches and ecosystem models overestimate total natural emissions. We build three contrasting emission scenarios — which differ in fossil fuel and microbial emissions — to explain the decadal variability in atmospheric methane levels detected, here and in previous studies, since 1985. Although uncertainties in emission trends do not allow definitive conclusions to be drawn, we show that the observed stabilization of methane levels between 1999 and 2006 can potentially be explained by decreasing-to-stable fossil fuel emissions, combined with stable-to-increasing microbial emissions. We show that a rise in natural wetland emissions and fossil fuel emissions probably accounts for the renewed increase in global methane levels after 2006, although the relative contribution of these two sources remains uncertain.
Lamarque, Jean-Francois, Larry W Horowitz, and Vaishali Naik, et al., February 2013: The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): overview and description of models, simulations and climate diagnostics. Geoscientific Model Development, DOI:10.5194/gmd-6-179-2013. Abstract
The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) consists of a series of timeslice experiments targeting the long-term changes in atmospheric composition between 1850 and 2100, with the goal of documenting radiative forcing and the associated composition changes. Here we introduce the various simulations performed under ACCMIP and the associated model output. The ACCMIP models have a wide range of horizontal and vertical resolutions, vertical extent, chemistry schemes and interaction with radiation and clouds. While anthropogenic and biomass burning emissions were specified for all time slices in the ACCMIP protocol, it is found that the natural emissions lead to a significant range in emissions, mostly for ozone precursors. The analysis of selected present-day climate diagnostics (precipitation, temperature, specific humidity and zonal wind) reveals biases consistent with state-of-the-art climate models. The model-to-model comparison of changes in temperature, specific humidity and zonal wind between 1850 and 2000 and between 2000 and 2100 indicates mostly consistent results, but with outliers different enough to possibly affect their representation of climate impact on chemistry.
Lee, Y-H, Larry W Horowitz, and Vaishali Naik, et al., March 2013: Evaluation of preindustrial to present-day black carbon and its albedo forcing from ACCMIP (Atmospheric Chemistry and Climate Model Intercomparison Project). Atmospheric Chemistry and Physics, 13(5), DOI:10.5194/acp-13-2607-2013. Abstract
As part of the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), we evaluate the historical black carbon (BC) aerosols simulated by 8 ACCMIP models against observations including 12 ice core records, long-term surface mass concentrations and recent Arctic BC snowpack measurements. We also estimate BC albedo forcing by performing additional simulations using offline models with prescribed meteorology from 1996–2000. We evaluated the vertical profile of BC snow concentrations from these offline simulations using the recent BC snowpack measurements.
Despite using the same BC emissions, the global BC burden differs by approximately a factor of 3 among models due to differences in aerosol removal parameterizations and simulated meteorology: 34 Gg to 103 Gg in 1850 and 82 Gg to 315 Gg in 2000. However, the global BC burden from preindustrial to present-day increases by 2.5–3 times with little variation among models, roughly matching the 2.5-fold increase in total BC emissions during the same period. We find a large divergence among models at both Northern Hemisphere (NH) and Southern Hemisphere (SH) high latitude regions for BC burden and at SH high latitude regions for deposition fluxes. The ACCMIP simulations match the observed BC surface mass concentrations well in Europe and North America except at Jungfraujoch and Ispra. However, the models fail to predict the Arctic BC seasonality due to severe underestimations during winter and spring. The simulated vertically resolved BC snow concentrations are, on average, within a factor of 2–3 of the BC snowpack measurements except for Greenland and the Arctic Ocean.
For the ice core evaluation, models tend to capture both the observed temporal trends and the magnitudes well at Greenland sites. However, models fail to predict the decreasing trend of BC depositions/ice-core concentrations from the 1950s to the 1970s in most Tibetan Plateau ice cores. The distinct temporal trend at the Tibetan Plateau ice cores indicates a strong influence from Western Europe, but the modeled BC increases in that period are consistent with the emission changes in Eastern Europe, the Middle East, South and East Asia. At the Alps site, the simulated BCsuggests a strong influence from Europe, which agrees with the Alps ice core observations. Models successfully simulate higher BC concentrations observed at Zuoqiupu during the non-monsoon season than monsoon season, but models underpredict BC in both seasons. Despite a large divergence in BC deposition at two Antarctic ice core sites, models are able to capture the relative increase from preindustrial to present-day seen in the ice cores.
In 2000 relative to 1850, globally annually averaged BC surface albedo forcing from the offline simulations ranges from 0.014 to 0.019 W m−2 among the ACCMIP models. Comparing offline and online BC albedo forcings computed by some of the same models, we find that the global annual mean can vary by up to a factor of two because of different aerosol models or different BC-snow parameterizations and snow cover. The spatial distributions of the offline BC albedo forcing in 2000 show especially high BC forcing (i.e. over 0.1 W m−2) over Manchuria, Karakoram, and most of the Former USSR. Models predict the highest global annual mean BC forcing in 1980 rather than 2000, mostly driven by the high fossil fuel and biofuel emissions in the Former USSR in 1980.
Employing the Geophysical Fluid Dynamics Laboratory (GFDL)'s fully-coupled chemistry-climate (ocean/atmosphere/land/sea ice) model (CM3) with an explicit physical representation of aerosol indirect effects (cloud-water droplet activation), we find that the dramatic emission reductions (35–80%) in anthropogenic aerosols and their precursors projected by Representative Concentration Pathway (RCP) 4.5 result in ~1°C of additional warming and ~0.1 mm day−1 of additional precipitation, both globally averaged, by the end of the 21st century. The impact of these reductions in aerosol emissions on simulated global mean surface temperature and precipitation becomes apparent by mid-21st century. Furthermore, we find that the aerosol emission reductions cause precipitation to increase in East and South Asia by ~1.0 mm day−1 through the 2nd half of the 21st century. Both the simulated temperature and precipitation responses in CM3 are significantly stronger than the previously simulated responses in our earlier climate model (CM2.1) that only considered direct radiative forcing by aerosols. We conclude that sulfate aerosol indirect effects greatly enhance the impacts of aerosols on surface temperature in CM3, while both direct and indirect effects from sulfate aerosols dominate the strong precipitation response, possibly with a small contribution from carbonaceous aerosols. Just as we found with the previous GFDL model, CM3 produces surface warming patterns that are uncorrelated with the spatial distribution of 21stcentury changes in aerosol loading. However, the largest precipitation increases in CM3 are co-located with the region of greatest aerosol decrease, in and downwind of Asia.
Biomass burning is one of the largest sources of trace gases and aerosols to the atmosphere, and has profound influence on tropospheric oxidants and radiative forcing. Using a fully coupled chemistry-climate model (GFDL AM3), we find that co-emission of trace gases and aerosol from present-day biomass burning increases the global tropospheric ozone burden by 5.1%, and decreases global mean OH by 6.3%. Gas and aerosol emissions combine to increase CH4 lifetime non-linearly. Heterogeneous processes are shown to contribute partly to the observed lower ΔO3/ΔCO ratios in northern high latitudes versus tropical regions. The radiative forcing from biomass burning is shown to vary non-linearly with biomass burning strength. At present-day emission levels, biomass burning produces a net radiative forcing of −0.19 W/m2 (−0.29 from short-lived species, mostly aerosol direct and indirect effects, +0.10 from CH4 and CH4-induced changes in O3 and stratospheric H2O), but increasing emissions to over 5 times present levels would result in a positive net forcing.
Nabat, Pierre, Larry W Horowitz, and Vaishali Naik, et al., May 2013: A 4-D climatology (1979–2009) of the monthly tropospheric aerosol optical depth distribution over the Mediterranean region from a comparative evaluation and blending of remote sensing and model products. Atmospheric Measurement Techniques, 6(5), DOI:10.5194/amt-6-1287-2013. Abstract
Since the 1980s several spaceborne sensors have been used to retrieve the aerosol optical depth (AOD) over the Mediterranean region. In parallel, AOD climatologies coming from different numerical model simulations are now also available, permitting to distinguish the contribution of several aerosol types to the total AOD. In this work, we perform a comparative analysis of this unique multi-year database in terms of total AOD and of its apportionment by the five main aerosol types (soil dust, sea-salt, sulfate, black and organic carbon). We use 9 different satellite-derived monthly AOD products: NOAA/AVHRR, SeaWiFS (2 products), TERRA/MISR, TERRA/MODIS, AQUA/MODIS, ENVISAT/MERIS, PARASOL/POLDER and MSG/SEVIRI, as well as 3 more historical datasets: NIMBUS7/CZCS, TOMS (onboard NIMBUS7 and Earth-Probe) and METEOSAT/MVIRI. Monthly model datasets include the aerosol climatology from Tegen et al. (1997), the climate-chemistry models LMDz-OR-INCA and RegCM-4, the multi-model mean coming from the ACCMIP exercise, and the reanalyses GEMS and MACC. Ground-based Level-2 AERONET AOD observations from 47 stations around the basin are used here to evaluate the model and satellite data. The sensor MODIS (on AQUA and TERRA) has the best average AOD scores over this region, showing a relevant spatio-temporal variability and highlighting high dust loads over Northern Africa and the sea (spring and summer), and sulfate aerosols over continental Europe (summer). The comparison also shows limitations of certain datasets (especially MERIS and SeaWiFS standard products). Models reproduce the main patterns of the AOD variability over the basin. The MACC reanalysis is the closest to AERONET data, but appears to underestimate dust over Northern Africa, where RegCM-4 is found closer to MODIS thanks to its interactive scheme for dust emissions. The vertical dimension is also investigated using the CALIOP instrument. This study confirms differences of vertical distribution between dust aerosols showing a large vertical spread, and other continental and marine aerosols which are confined in the boundary layer. From this compilation, we propose a 4-D blended product from model and satellite data, consisting in monthly time series of 3-D aerosol distribution at a 50 km horizontal resolution over the Euro-Mediterranean marine and continental region for the 2003–2009 period. The product is based on the total AOD from AQUA/MODIS, apportioned into sulfates, black and organic carbon from the MACC reanalysis, and into dust and sea-salt aerosols from RegCM-4 simulations, which are distributed vertically based on CALIOP climatology. We extend the 2003–2009 reconstruction to the past up to 1979 using the 2003–2009 average and applying the decreasing trend in sulfate aerosols from LMDz-OR-INCA, whose AOD trends over Europe and the Mediterranean are median among the ACCMIP models. Finally optical properties of the different aerosol types in this region are proposed from Mie calculations so that this reconstruction can be included in regional climate models for aerosol radiative forcing and aerosol-climate studies.
Naik, Vaishali, A Voulgarakis, Arlene M Fiore, Larry W Horowitz, Jean-Francois Lamarque, and Meiyun Lin, et al., May 2013: Preindustrial to present day changes in tropospheric hydroxyl radical and methane lifetime from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). Atmospheric Chemistry and Physics, 13(10), DOI:10.5194/acp-13-5277-2013. Abstract
We have analysed results from 17 global models, participating in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), to explore trends in hydroxyl radical concentration (OH) and methane (CH4) lifetime since preindustrial times (1850) and gain a better understanding of their key drivers. For the present day (2000), the models tend to simulate higher OH abundances in the Northern Hemisphere versus Southern Hemisphere. Evaluation of simulated carbon monoxide concentrations, the primary sink for OH, against observations suggests low biases in the Northern Hemisphere that may contribute to the high north-south OH asymmetry in the models. A comparison of modelled and observed methyl chloroform lifetime suggests that the present day global multi-model mean OH concentration is slightly overestimated. Despite large regional changes, the modelled global mean OH concentration is roughly constant over the past 150 yr, due to concurrent increases in OH sources (humidity, tropospheric ozone, and NOx emissions), together with decreases in stratospheric ozone and increase in tropospheric temperature, compensated by increases in OH sinks (methane abundance, carbon monoxide and non-methane volatile organic carbon (NMVOC) emissions). The large intermodel diversity in the sign and magnitude of OH and methane lifetime changes over this period reflects differences in the relative importance of chemical and physical drivers of OH within each model. For the 1980 to 2000 period, we find that climate warming and a slight increase in mean OH leads to a 4.3 ± 1.9% decrease in the methane lifetime. Analysing sensitivity simulations performed by 10 models, we find that preindustrial to present day climate change decreased the methane lifetime by about 4 months, representing a negative feedback on the climate system. Further, using a subset of the models, we find that global mean OH increased by 46.4 ± 12.2% in response to preindustrial to present day anthropogenic NOx emission increases, and decreased by 17.3 ± 2.3%, 7.6 ± 1.5%, and 3.1 ± 3.0% due to methane burden, and anthropogenic CO, and NMVOC emissions increases, respectively.
We describe and evaluate atmospheric chemistry in the newly developed Geophysical Fluid Dynamics Laboratory chemistry-climate model (GFDL AM3) and apply it to investigate the net impact of preindustrial (PI) to present (PD) changes in short-lived pollutant emissions (ozone precursors, sulfur dioxide, and carbonaceous aerosols) and methane concentration on atmospheric composition and climate forcing. The inclusion of online troposphere-stratosphere interactions, gas-aerosol chemistry, and aerosol-cloud interactions (including direct and indirect aerosol radiative effects) in AM3 enables a more complete representation of interactions among short-lived species, and thus their net climate impact, than was considered in previous climate assessments. The base AM3 simulation, driven with observed sea surface temperature (SST) and sea ice cover (SIC) over the period 1981–2007, generally reproduces the observed mean magnitude, spatial distribution, and seasonal cycle of tropospheric ozone and carbon monoxide. The global mean aerosol optical depth in our base simulation is within 5% of satellite measurements over the 1982–2006 time period. We conduct a pair of simulations in which only the short-lived pollutant emissions and methane concentrations are changed from PI (1860) to PD (2000) levels (i.e., SST, SIC, greenhouse gases, and ozone depleting substances are held at PD levels). From the PI to PD, we find that changes in short-lived pollutant emissions and methane have caused the tropospheric ozone burden to increase by 39% and the global burdens of sulfate, black carbon and organic carbon to increase by factors of 3, 2.4 and 1.4, respectively. Tropospheric hydroxyl concentration decreases by 7%, showing that increases in OH sinks (methane, carbon monoxide, non-methane volatile organic compounds, and sulfur dioxide) dominate over sources (ozone and nitrogen oxides) in the model. Combined changes in tropospheric ozone and aerosols cause a net negative top-of-the-atmosphere radiative forcing perturbation (−1.05 Wm-2) indicating that the negative forcing (direct plus indirect) from aerosol changes dominates over the positive forcing due to ozone increases, thus masking nearly half of the PI to PD positive forcing from long-lived greenhouse gases globally, consistent with other current generation chemistry-climate models.
The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) examined the short-lived drivers of climate change in current climate models. Here we evaluate the 10 ACCMIP models that included aerosols, 8 of which also participated in the Coupled Model Intercomparison Project phase 5 (CMIP5).
The models reproduce present-day total aerosol optical depth (AOD) relatively well, though many are biased low. Contributions from individual aerosol components are quite different, however, and most models underestimate east Asian AOD. The models capture most 1980–2000 AOD trends well, but underpredict increases over the Yellow/Eastern Sea. They strongly underestimate absorbing AOD in many regions.
We examine both the direct radiative forcing (RF) and the forcing including rapid adjustments (effective radiative forcing; ERF, including direct and indirect effects). The models' all-sky 1850 to 2000 global mean annual average total aerosol RF is (mean; range) −0.26 W m−2; −0.06 to −0.49 W m−2. Screening based on model skill in capturing observed AOD yields a best estimate of −0.42 W m−2; −0.33 to −0.50 W m−2, including adjustment for missing aerosol components in some models. Many ACCMIP and CMIP5 models appear to produce substantially smaller aerosol RF than this best estimate. Climate feedbacks contribute substantially (35 to −58%) to modeled historical aerosol RF. The 1850 to 2000 aerosol ERF is −1.17 W m−2; −0.71 to −1.44 W m−2. Thus adjustments, including clouds, typically cause greater forcing than direct RF. Despite this, the multi-model spread relative to the mean is typically the same for ERF as it is for RF, or even smaller, over areas with substantial forcing. The largest 1850 to 2000 negative aerosol RF and ERF values are over and near Europe, south and east Asia and North America. ERF, however, is positive over the Sahara, the Karakoram, high Southern latitudes and especially the Arctic.
Global aerosol RF peaks in most models around 1980, declining thereafter with only weak sensitivity to the Representative Concentration Pathway (RCP). One model, however, projects approximately stable RF levels, while two show increasingly negative RF due to nitrate (not included in most models). Aerosol ERF, in contrast, becomes more negative during 1980 to 2000. During this period, increased Asian emissions appear to have a larger impact on aerosol ERF than European and North American decreases due to their being upwind of the large, relatively pristine Pacific Ocean. There is no clear relationship between historical aerosol ERF and climate sensitivity in the CMIP5 subset of ACCMIP models. In the ACCMIP/CMIP5 models, historical aerosol ERF of about −0.8 to −1.5 W m−2 is most consistent with observed historical warming. Aerosol ERF masks a large portion of greenhouse forcing during the late 20th and early 21st century at the global scale. Regionally, aerosol ERF is so large that net forcing is negative over most industrialized and biomass burning regions through 1980, but remains strongly negative only over east and southeast Asia by 2000. Net forcing is strongly positive by 1980 over most deserts, the Arctic, Australia, and most tropical oceans. Both the magnitude of and area covered by positive forcing expand steadily thereafter.
Silva, R A., Larry W Horowitz, and Vaishali Naik, et al., September 2013: Global premature mortality due to anthropogenic outdoor air pollution and the contribution of past climate change. Environmental Research Letters, 8(3), DOI:10.1088/1748-9326/8/3/034005. Abstract
Increased concentrations of ozone and fine particulate matter (PM2.5) since preindustrial times reflect increased emissions, but also contributions of past climate change. Here we use modeled concentrations from an ensemble of chemistry–climate models to estimate the global burden of anthropogenic outdoor air pollution on present-day premature human mortality, and the component of that burden attributable to past climate change. Using simulated concentrations for 2000 and 1850 and concentration–response functions (CRFs), we estimate that, at present, 470 000 (95% confidence interval, 140 000 to 900 000) premature respiratory deaths are associated globally and annually with anthropogenic ozone, and 2.1 (1.3 to 3.0) million deaths with anthropogenic PM2.5-related cardiopulmonary diseases (93%) and lung cancer (7%). These estimates are smaller than ones from previous studies because we use modeled 1850 air pollution rather than a counterfactual low concentration, and because of different emissions. Uncertainty in CRFs contributes more to overall uncertainty than the spread of model results. Mortality attributed to the effects of past climate change on air quality is considerably smaller than the global burden: 1500 (−20 000 to 27 000) deaths yr−1 due to ozone and 2200 (−350 000 to 140 000) due to PM2.5. The small multi-model means are coincidental, as there are larger ranges of results for individual models, reflected in the large uncertainties, with some models suggesting that past climate change has reduced air pollution mortality.
Stevenson, David S., Vaishali Naik, and Larry W Horowitz, et al., March 2013: Tropospheric ozone changes, radiative forcing and attribution to emissions in the Atmospheric Chemistry and Climate Model Inter-comparison Project (ACCMIP). Atmospheric Chemistry and Physics, 13(6), DOI:10.5194/acp-13-3063-2013. Abstract
Ozone (O3) from 17 atmospheric chemistry models taking part in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) has been used to calculate tropospheric ozone radiative forcings (RFs). We calculate a~value for the pre-industrial (1750) to present-day (2010) tropospheric ozone RF of 0.40 W m−2. The model range of pre-industrial to present-day changes in O3 produces a spread (±1 standard deviation) in RFs of ±17%. Three different radiation schemes were used – we find differences in RFs between schemes (for the same ozone fields) of ±10%. Applying two different tropopause definitions gives differences in RFs of ±3%. Given additional (unquantified) uncertainties associated with emissions, climate-chemistry interactions and land-use change, we estimate an overall uncertainty of ±30% for the tropospheric ozone RF. Experiments carried out by a subset of six models attribute tropospheric ozone RF to increased emissions of methane (47%), nitrogen oxides (29%), carbon monoxide (15%) and non-methane volatile organic compounds (9%); earlier studies attributed more of the tropospheric ozone RF to methane and less to nitrogen oxides. Normalising RFs to changes in tropospheric column ozone, we find a global mean normalised RF of 0.042 W m−2 DU−1, a value similar to previous work. Using normalised RFs and future tropospheric column ozone projections we calculate future tropospheric ozone RFs (W m−2; relative to 1850 – add 0.04 W m−2 to make relative to 1750) for the Representative Concentration Pathways in 2030 (2100) of: RCP2.6: 0.31 (0.16); RCP4.5: 0.38 (0.26); RCP6.0: 0.33 (0.24); and RCP8.5: 0.42 (0.56). Models show some coherent responses of ozone to climate change: decreases in the tropical lower troposphere, associated with increases in water vapour; and increases in the sub-tropical to mid-latitude upper troposphere, associated with increases in lightning and stratosphere-to-troposphere transport.
Results from simulations performed for the Atmospheric Chemistry and Climate Modeling Intercomparison Project (ACCMIP) are analysed to examine how OH and methane lifetime may change from present-day to the future, under different climate and emissions scenarios. Present-day (2000) mean tropospheric chemical lifetime derived from the ACCMIP multi-model mean is 9.8 ± 1.6 yr, lower than a recent observationally-based estimate, but with a similar range to previous multi-model estimates. Future model projections are based on the four Representative Concentration Pathways (RCPs), and the results also exhibit a~large range. Decreases in global methane lifetime of 4.5 ± 9.1% are simulated for the scenario with lowest radiative forcing by 2100 (RCP 2.6), while increases of 8.5 ± 10.4% are simulated for the scenario with highest radiative forcing (RCP 8.5). In this scenario, the key driver of the evolution of OH and methane lifetime is methane itself, since its concentration more than doubles by 2100, and it consumes much of the OH that exists in the troposphere. Stratospheric ozone recovery, which drives tropospheric OH decreases through photolysis modifications, also plays a~partial role. In the other scenarios, where methane changes are less drastic, the interplay between various competing drivers leads to smaller and more diverse OH and methane lifetime responses, which are difficult to attribute. For all scenarios, regional OH changes are even more variable, with the most robust feature being the large decreases over the remote oceans in RCP 8.5. Through a~regression analysis, we suggest that differences in emissions of non-methane volatile organic compounds and in the simulation of photolysis rates may be the main factors causing the differences in simulated present-day OH and methane lifetime. Diversity in predicted changes between present-day and future was found to be associated more strongly with differences in modelled climate changes, specifically global temperature and humidity. Finally, through perturbation experiments we calculated an OH feedback factor (F) of 1.29 from present-day conditions (1.65 from 2100 RCP 8.5 conditions) and a~climate feedback on methane lifetime of 0.33 ± 0.13 yr K−1, on average.
West, J J., Vaishali Naik, and Larry W Horowitz, et al., October 2013: Co-benefits of mitigating global greenhouse gas emissions for future air quality and human health. Nature Climate Change, 3(10), DOI:10.1038/nclimate2009. Abstract
Actions to reduce greenhouse gas (GHG) emissions often reduce co-emitted air pollutants, bringing co-benefits for air quality and human health. Past studies typically evaluated near-term and local co-benefits, neglecting the long-range transport of air pollutants, long-term demographic changes, and the influence of climate change on air quality. Here we simulate the co-benefits of global GHG reductions on air quality and human health using a global atmospheric model and consistent future scenarios, via two mechanisms: reducing co-emitted air pollutants, and slowing climate change and its effect on air quality. We use new relationships between chronic mortality and exposure to fine particulate matter and ozone, global modelling methods and new future scenarios. Relative to a reference scenario, global GHG mitigation avoids 0.5±0.2, 1.3±0.5 and 2.2±0.8 million premature deaths in 2030, 2050 and 2100. Global average marginal co-benefits of avoided mortality are US$50–380 per tonne of CO2, which exceed previous estimates, exceed marginal abatement costs in 2030 and 2050, and are within the low range of costs in 2100. East Asian co-benefits are 10–70 times the marginal cost in 2030. Air quality and health co-benefits, especially as they are mainly local and near-term, provide strong additional motivation for transitioning to a low-carbon future.
Young, Paul J., Vaishali Naik, and Larry W Horowitz, et al., February 2013: Pre-industrial to end 21st century projections of tropospheric ozone from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). Atmospheric Chemistry and Physics, 13(4), DOI:10.5194/acp-13-2063-2013. Abstract
Present day tropospheric ozone and its changes between 1850 and 2100 are considered, analysing 15 global models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The multi-model mean compares well against present day observations. The seasonal cycle correlates well, except for some locations in the tropical upper troposphere. Most (75%) of the models are encompassed with a range of global mean tropospheric ozone column estimates from satellite data, although there is a suggestion of a high bias in the Northern Hemisphere and a low bias in the Southern Hemisphere. Compared to the present day multi-model mean tropospheric ozone burden of 337 Tg, the multi-model mean burden for 1850 time slice is ~ 30% lower. Future changes were modelled using emissions and climate projections from four Representative Concentration Pathways (RCPs). Compared to 2000, the relative changes for the tropospheric ozone burden in 2030 (2100) for the different RCPs are: −5% (−22%) for RCP2.6, 3% (−8%) for RCP4.5, 0% (−9%) for RCP6.0, and 5% (15%) for RCP8.5. Model agreement on the magnitude of the change is greatest for larger changes. Reductions in precursor emissions are common across the RCPs and drive ozone decreases in all but RCP8.5, where doubled methane and a larger stratospheric influx increase ozone. Models with high ozone abundances for the present day also have high ozone levels for the other time slices, but there are no models consistently predicting large or small changes. Spatial patterns of ozone changes are well correlated across most models, but are notably different for models without time evolving stratospheric ozone concentrations. A unified approach to ozone budget specifications is recommended to help future studies attribute ozone changes and inter-model differences more clearly.
Emissions of air pollutants and their precursors determine regional air quality and can alter climate. Climate change can perturb the long-range transport, chemical processing, and local meteorology that influence air pollution. We review the implications of projected changes in methane (CH4), ozone precursors (O3), and aerosols for climate (expressed in terms of the radiative forcing metric or changes in global surface temperature) and hemispheric-to-continental scale air quality. Reducing the O3 precursor CH4 would slow near-term warming by decreasing both CH4 and tropospheric O3. Uncertainty remains as to the net climate forcing from anthropogenic nitrogen oxide (NOx) emissions, which increase tropospheric O3 (warming) but also increase aerosols and decrease CH4 (both cooling). Anthropogenic emissions of carbon monoxide (CO) and non-CH4 volatile organic compounds (NMVOC) warm by increasing both O3 and CH4. Radiative impacts from secondary organic aerosols (SOA) are poorly understood. Black carbon emission controls, by reducing the absorption of sunlight in the atmosphere and on snow and ice, have the potential to slow near-term warming, but uncertainties in coincident emissions of reflective (cooling) aerosols and poorly constrained cloud indirect effects confound robust estimates of net climate impacts. Reducing sulfate and nitrate aerosols would improve air quality and lessen interference with the hydrologic cycle, but lead to warming. A holistic and balanced view is thus needed to assess how air pollution controls influence climate; a first step towards this goal involves estimating net climate impacts from individual emission sectors. Modeling and observational analyses suggest a warming climate degrades air quality (increasing surface O3 and particulate matter) in many populated regions, including during pollution episodes. Prior Intergovernmental Panel on Climate Change (IPCC) scenarios (SRES) allowed unconstrained growth, whereas the Representative Concentration Pathway (RCP) scenarios assume uniformly an aggressive reduction, of air pollutant emissions. New estimates from the current generation of chemistry–climate models with RCP emissions thus project improved air quality over the next century relative to those using the IPCC SRES scenarios. These two sets of projections likely bracket possible futures. We find that uncertainty in emission-driven changes in air quality is generally greater than uncertainty in climate-driven changes. Confidence in air quality projections is limited by the reliability of anthropogenic emission trajectories and the uncertainties in regional climate responses, feedbacks with the terrestrial biosphere, and oxidation pathways affecting O3 and SOA.
Fry, M, Vaishali Naik, J Jason West, M Daniel Schwarzkopf, and Arlene M Fiore, et al., April 2012: The influence of ozone precursor emissions from four world regions on tropospheric composition and radiative climate forcing. Journal of Geophysical Research: Atmospheres, 117, D07306, DOI:10.1029/2011JD017134. Abstract
Ozone (O3) precursor emissions influence regional and global climate and air quality through changes in tropospheric O3 and oxidants, which also influence methane (CH4) and sulfate aerosols (SO42-). We examine changes in the tropospheric composition of O3, CH4, SO42- and global net radiative forcing (RF) for 20% reductions in global CH4 burden and in anthropogenic O3 precursor emissions (NOx, NMVOC, and CO) from four regions (East Asia, Europe and Northern Africa, North America, and South Asia) using the Task Force on Hemispheric Transport of Air Pollution Source-Receptor global chemical transport model (CTM) simulations, assessing uncertainty (mean {plus minus}1 standard deviation) across multiple CTMs. We evaluate steady-state O3 responses, including long-term feedbacks via CH4. With a radiative transfer model that includes greenhouse gases and the aerosol direct effect, we find that regional NOx reductions produce global, annually averaged positive net RFs (0.2 {plus minus}0.6 to 1.7 {plus minus}2 mWm-2/TgN yr-1), with some variation among models. Negative net RFs result from reductions in global CH4 (-162.6 {plus minus}2 mWm-2 for a change from 1760 to 1408 ppbv CH4) and regional NMVOC (-0.4 {plus minus}0.2 to -0.7 {plus minus}0.2 mWm-2/TgC yr-1) and CO emissions (-0.13 {plus minus}0.02 to -0.15 {plus minus}0.02 mWm-2/TgCO yr-1). Including the effect of O3 on CO2 uptake by vegetation, likely makes these net RFs more negative by -1.9 to -5.2 mWm-2/TgN yr-1, -0.2 to -0.7 mWm-2/TgC yr-1, and -0.02 to -0.05 mWm-2/TgCO yr-1. Net RF impacts reflect the distribution of concentration changes, where RF is affected locally by changes in SO42-, regionally to hemispherically by O3, and globally by CH4. Global annual average SO42- responses to oxidant changes range from 0.4 {plus minus}2.6 to -1.9 {plus minus}1.3 Gg for NOx reductions, 0.1 {plus minus}1.2 to -0.9 {plus minus}0.8 Gg for NMVOC reductions, and -0.09 {plus minus}0.5 to -0.9 {plus minus}0.8 Gg for CO reductions, suggesting additional research is needed. The 100-year global warming potentials (GWP100) are calculated for the global CH4 reduction (20.9 {plus minus}3.7 without stratospheric O3 or water vapor, 24.2 {plus minus}4.2 including those components), and for the regional NOx, NMVOC, and CO reductions (-18.7 {plus minus}25.9 to -1.9 {plus minus}8.7 for NOx, 4.8 {plus minus}1.7 to 8.3 {plus minus}1.9 for NMVOC, and 1.5 {plus minus}0.4 to 1.7 {plus minus}0.5 for CO). Variation in GWP100 for NOx, NMVOC, and CO suggests that regionally-specific GWPs may be necessary and could support the inclusion of O3 precursors in future policies that address air quality and climate change simultaneously. Both global net RF and GWP100 are more sensitive to NOx and NMVOC reductions from South Asia than the other three regions.
With a more-than-doubling in the atmospheric abundance of the potent greenhouse gas methane (CH4) since preindustrial times, and indications of renewed growth following a leveling off in recent years, questions arise as to future trends and resulting climate and public health impacts from continued growth without mitigation. Changes in atmospheric methane lifetime are determined by factors which regulate the abundance of OH, the primary methane removal mechanism, including changes in CH4 itself. We investigate the role of emissions of short-lived species and climate in determining the evolution of tropospheric methane lifetime in a suite of historical (1860�2005) and Representative Concentration Pathway (RCP) simulations (2006�2100), conducted with the Geophysical Fluid Dynamics Laboratory (GFDL) fully coupled chemistry-climate model (CM3). From preindustrial to present, CM3 simulates an overall 5% increase in CH4 lifetime due to a doubling of the methane burden which offsets coincident increases in nitrogen oxide (NOx) emissions. Over the last two decades, however, the methane lifetime declines steadily, coinciding with the most rapid climate warming and observed slow-down in CH4 growth rates, reflecting a possible negative feedback through the CH4 sink. The aerosol indirect effect plays a significant role in the CM3 climate and thus in the future evolution of the methane lifetime, due to the rapid projected decline of aerosols under all four RCPs. In all scenarios, the methane lifetime decreases (by 5�13%) except for the most extreme warming case (RCP8.5), where it increases by 4% due to the near-doubling of the CH4 abundance, reflecting a positive feedback on the climate system. In the RCP4.5 scenario changes in short-lived climate forcing agents reinforce climate warming and enhance OH, leading to a more-than-doubling of the decrease in methane lifetime from 2006 to 2100 relative to a simulation in which only well-mixed greenhouse gases are allowed to change along the RCP4.5 scenario (13% vs. 5%) Future work should include process-based studies to better understand and elucidate the individual mechanisms controlling methane lifetime.
Many prior studies clearly document episodic Asian pollution in the western U.S.
free troposphere. Here, we examine the mechanisms involved in the transport of Asian
pollution plumes into western U.S. surface air through an integrated analysis of in situ
and satellite measurements in May–June 2010 with a new global high-resolution
(50 50 km2) chemistry-climate model (GFDL AM3). We find that AM3 with
full stratosphere-troposphere chemistry nudged to reanalysis winds successfully
reproduces observed sharp ozone gradients above California, including the interleaving
and mixing of Asian pollution and stratospheric air associated with complex interactions of
midlatitude cyclone air streams. Asian pollution descends isentropically behind cold fronts;
at 800 hPa a maximum enhancement to ozone occurs over the southwestern U.S.,
including the densely populated Los Angeles Basin. During strong episodes, Asian
emissions can contribute 8–15 ppbv ozone in the model on days when observed daily
maximum 8-h average ozone (MDA8 O3) exceeds 60 ppbv. We find that in the absence
of Asian anthropogenic emissions, 20% of MDA8 O3 exceedances of 60 ppbv in the model
would not have occurred in the southwestern USA. For a 75 ppbv threshold, that
statistic increases to 53%. Our analysis indicates the potential for Asian emissions to
contribute to high-O3 episodes over the high-elevation western USA, with implications
for attaining more stringent ozone standards in this region. We further demonstrate a
proof-of-concept approach using satellite CO column measurements as a qualitative early
warning indicator to forecast Asian ozone pollution events in the western U.S. with
lead times of 1–3 days.
The published literature debates the extent to which naturally occurring stratospheric ozone intrusions reach the surface and contribute to exceedances of the U.S. National Ambient Air Quality Standard (NAAQS) for ground-level ozone (75 ppbv implemented in 2008). Analysis of ozonesondes, lidar, and surface measurements over the western U.S. from April to June 2010 show that a global high-resolution (~50x50 km2) chemistry-climate model (GFDL AM3) captures the observed layered features and sharp ozone gradients of deep stratospheric intrusions, representing a major improvement over previous chemical transport models. Thirteen intrusions enhanced total daily maximum 8-hour average (MDA8) ozone to ~70-86 ppbv at surface sites. With a stratospheric ozone tracer defined relative to a dynamically-varying tropopause, we find that stratospheric intrusions can episodically increase surface MDA8 ozone by 20-40 ppbv (all model estimates are bias corrected), including on days when observed ozone exceeds the NAAQS threshold. These stratospheric intrusions elevated background ozone concentrations (estimated by turning off North American anthropogenic emissions in the model) to MDA8 values of 60-75 ppbv. At high-elevation western U.S. sites, the 25th-75th percentile of the stratospheric contribution is 15-25 ppbv when observed MDA8 ozone is 60-70 ppbv, and increases to ~17-40 ppbv for the 70-85 ppbv range. These estimates, up to 2-3 times greater than previously reported, indicate a major role for stratospheric intrusions in contributing to springtime high-O3 events over the high-altitude western U.S., posing a challenge for staying below the ozone NAAQS threshold, particularly if a value in the 60-70 ppbv range were to be adopted.
We use long-term, coincident O3 and temperature measurements at the regionally representative US Environmental Protection Agency Clean Air Status and Trends Network (CASTNet) over the eastern US from 1988 through 2009 to characterize the surface O3 response to year-to-year fluctuations in weather, for the purpose of evaluating global chemistry-climate models. We first produce a monthly climatology for each site over all available years, defined as the slope of the best-fit line (mO3-T) between monthly average values of maximum daily 8-hour average (MDA8) O3 and monthly average values of daily maximum surface temperature (Tmax). Applying two distinct statistical approaches to aggregate the site-specific measurements to the regional scale, we find that summertime mO3-T is 3–6 ppb K−1 (r = 0.5–0.8) over the Northeast, 3–4 ppb K−1 (r = 0.5–0.9) over the Great Lakes, and 3–6 ppb K−1 (r = 0.2–0.8) over the Mid-Atlantic. The Geophysical Fluid Dynamics Laboratory (GFDL) Atmospheric Model version 3 (AM3) global chemistry-climate model generally captures the seasonal variations in correlation coefficients and mO3-T despite biases in both monthly mean summertime MDA8 O3 (up to +10 to +30 ppb) and daily Tmax (up to +5 K) over the eastern US. During summer, GFDL AM3 reproduces mO3-T over the Northeast (mO3-T = 2–6 ppb K−1; r = 0.6–0.9), but underestimates mO3-Tby 4 ppb K−1 over the Mid-Atlantic, in part due to excessively warm temperatures above which O3 production saturates in the model. Combining Tmax biases in GFDL AM3 with an observation-based mO3-T estimate of 3 ppb K−1 implies that temperature biases could explain up to 5–15 ppb of the MDA8 O3 bias in August and September though correcting for excessively cool temperatures would worsen the O3 bias in June. We underscore the need for long-term, coincident measurements of air pollution and meteorological variables to develop process-level constraints for evaluating chemistry-climate models used to project air quality responses to climate change.
The Geophysical Fluid Dynamics Laboratory (GFDL) has developed a coupled general circulation model (CM3) for atmosphere, oceans, land, and sea ice. The goal of CM3 is to address emerging issues in climate change, including aerosol-cloud interactions, chemistry-climate interactions, and coupling between the troposphere and stratosphere. The model is also designed to serve as the physical-system component of earth-system models and models for decadal prediction in the near-term future, for example, through improved simulations in tropical land precipitation relative to earlier-generation GFDL models. This paper describes the dynamical core, physical parameterizations, and basic simulation characteristics of the atmospheric component (AM3) of this model.
Relative to GFDL AM2, AM3 includes new treatments of deep and shallow cumulus convection, cloud-droplet activation by aerosols, sub-grid variability of stratiform vertical velocities for droplet activation, and atmospheric chemistry driven by emissions with advective, convective, and turbulent transport. AM3 employs a cubed-sphere implementation of a finite-volume dynamical core and is coupled to LM3, a new land model with eco-system dynamics and hydrology.
Most basic circulation features in AM3 are simulated as realistically, or more so, than in AM2. In particular, dry biases have been reduced over South America. In coupled mode, the simulation of Arctic sea ice concentration has improved. AM3 aerosol optical depths, scattering properties, and surface clear-sky downward shortwave radiation are more realistic than in AM2. The simulation of marine stratocumulus decks and the intensity distributions of precipitation remain problematic, as in AM2.
The last two decades of the 20th century warm in CM3 by .32°C relative to 1881-1920. The Climate Research Unit (CRU) and Goddard Institute for Space Studies analyses of observations show warming of .56°C and .52°C, respectively, over this period. CM3 includes anthropogenic cooling by aerosol cloud interactions, and its warming by late 20th century is somewhat less realistic than in CM2.1, which warmed .66°C but did not include aerosol cloud interactions. The improved simulation of the direct aerosol effect (apparent in surface clear-sky downward radiation) in CM3 evidently acts in concert with its simulation of cloud-aerosol interactions to limit greenhouse gas warming in a way that is consistent with observed global temperature changes.
Lamarque, Jean-Francois, and Vaishali Naik, et al., August 2010: Historical (1850–2000) gridded anthropogenic and biomass burning emissions of reactive gases and aerosols: methodology and application. Atmospheric Chemistry and Physics, 10(15), DOI:10.5194/acp-10-7017-2010. Abstract
We present and discuss a new dataset of gridded emissions covering the historical period (1850–2000) in decadal increments at a horizontal resolution of 0.5° in latitude and longitude. The primary purpose of this inventory is to provide consistent gridded emissions of reactive gases and aerosols for use in chemistry model simulations needed by climate models for the Climate Model Intercomparison Program #5 (CMIP5) in support of the Intergovernmental Panel on Climate Change (IPCC) Fifth Assessment report (AR5). Our best estimate for the year 2000 inventory represents a combination of existing regional and global inventories to capture the best information available at this point; 40 regions and 12 sectors are used to combine the various sources. The historical reconstruction of each emitted compound, for each region and sector, is then forced to agree with our 2000 estimate, ensuring continuity between past and 2000 emissions. Simulations from two chemistry-climate models are used to test the ability of the emission dataset described here to capture long-term changes in atmospheric ozone, carbon monoxide and aerosol distributions. The simulated long-term change in the Northern mid-latitudes surface and mid-troposphere ozone is not quite as rapid as observed. However, stations outside this latitude band show much better agreement in both present-day and long-term trend. The model simulations indicate that the concentration of carbon monoxide is underestimated at the Mace Head station; however, the long-term trend over the limited observational period seems to be reasonably well captured. The simulated sulfate and black carbon deposition over Greenland is in very good agreement with the ice-core observations spanning the simulation period. Finally, aerosol optical depth and additional aerosol diagnostics are shown to be in good agreement with previously published estimates and observations.
Energy security and climate change concerns have led to the promotion of biomass-derived ethanol, an oxygenated volatile organic compound (OVOC), as a substitute for fossil fuels. Although ethanol is ubiquitous in the troposphere, our knowledge of its current atmospheric budget and distribution is limited. Here, for the first time we use a global chemical transport model in conjunction with atmospheric observations to place constraints on the ethanol budget, noting that additional measurements of ethanol (and its precursors) are still needed to enhance confidence in our estimated budget. Global sources of ethanol in the model include 5.0 Tg yr−1 from industrial sources and biofuels, 9.2 Tg yr−1 from terrestrial plants, ~0.5 Tg yr−1 from biomass burning, and 0.05 Tg yr−1 from atmospheric reactions of the ethyl peroxy radical (C2H5O2) with itself and with the methyl peroxy radical (CH3O2). The resulting atmospheric lifetime of ethanol in the model is 2.8 days. Gas-phase oxidation by the hydroxyl radical (OH) is the primary global sink of ethanol in the model (65%), followed by dry deposition (25%), and wet deposition (10%). Over continental areas, ethanol concentrations predominantly reflect direct anthropogenic and biogenic emission sources. Uncertainty in the biogenic ethanol emissions, estimated at a factor of three, may contribute to the 50% model underestimate of observations in the North American boundary layer. Current levels of ethanol measured in remote regions are an order of magnitude larger than those in the model, suggesting a major gap in understanding. Stronger constraints on the budget and distribution of ethanol and OVOCs are a critical step towards assessing the impacts of increasing the use of ethanol as a fuel.
Saikawa, E, Vaishali Naik, Larry W Horowitz, J Liu, and D L Mauzerall, June 2009: Present and potential future contributions of sulfate, black and organic carbon aerosols from China to global air quality, premature mortality and radiative forcing. Atmospheric Environment, 43(17), DOI:10.1016/j.atmosenv.2009.02.017. Abstract
Aerosols are harmful to human health and have both direct and indirect effects on climate. China is a major contributor to global emissions of sulfur dioxide (SO2), a sulfate (SO42−) precursor, organic carbon (OC), and black carbon (BC) aerosols. Although increasingly examined, the effect of present and potential future levels of these emissions on global premature mortality and climate change has not been well quantified. Through both direct radiative effects and indirect effects on clouds, SO42− and OC exert negative radiative forcing (cooling) while BC exerts positive forcing (warming). We analyze the effect of China's emissions of SO2, SO42−, OC and BC in 2000 and for three emission scenarios in 2030 on global surface aerosol concentrations, premature mortality, and radiative forcing (RF). Using global models of chemical transport (MOZART-2) and radiative transfer (GFDL RTM), and combining simulation results with gridded population data, mortality rates, and concentration–response relationships from the epidemiological literature, we estimate the contribution of Chinese aerosols to global annual premature mortality and to RF in 2000 and 2030. In 2000, we estimate these aerosols cause approximately 470 000 premature deaths in China and an additional 30 000 deaths globally. In 2030, aggressive emission controls lead to a 50% reduction in premature deaths from the 2000 level to 240 000 in China and 10 000 elsewhere, while under a high emissions scenario premature deaths increase 50% from the 2000 level to 720 000 in China and to 40 000 elsewhere. Because the negative RF from SO42− and OC is larger than the positive forcing from BC, Chinese aerosols lead to global net direct RF of −74 mW m−2 in 2000 and between −15 and −97 mW m−2 in 2030 depending on the emissions scenario. Our analysis indicates that increased effort to reduce greenhouse gases is essential to address climate change as China's anticipated reduction of aerosols will result in the loss of net negative radiative forcing.
Observations and models
demonstrate that ozone and its precursors can be transported between
continents and across oceans. We model the influences of 10% reductions in
anthropogenic nitrogen oxide (NOx) emissions from each of nine
world regions on surface ozone air quality in that region and all other
regions. In doing so, we quantify the relative importance of long-range
transport between all source-receptor pairs, for direct short-term ozone
changes. We find that for population-weighted concentrations during the
three-month "ozone-season", the strongest inter-regional influences are from
Europe to the Former Soviet Union, East Asia to Southeast Asia, and Europe
to Africa. The largest influences per unit of NOx reduced,
however, are seen for source regions in the tropics and Southern Hemisphere,
which we attribute mainly to greater sensitivity to changes in NOx
in the lower troposphere, and secondarily to increased vertical convection
to the free troposphere in tropical regions, allowing pollutants to be
transported further. Results show, for example, that NOx
reductions in North America are ~20% as effective per unit NOx in
reducing ozone in Europe during summer, as NOx reductions from
Europe itself. Reducing anthropogenic emissions of non-methane volatile
organic compounds (NMVOCs) and carbon monoxide (CO) by 10% in selected
regions, can have as large an impact on long-range ozone transport as NOx
reductions, depending on the source region. We find that for many
source-receptor pairs, the season of greatest long-range influence does not
coincide with the season when ozone is highest in the receptor region.
Reducing NOx emissions in most source regions causes a larger
decrease in export of ozone from the source region than in ozone production
outside of the source region.
West, J J., Vaishali Naik, Larry W Horowitz, and Arlene M Fiore, August 2009: Effect of regional precursor emission controls on long-range ozone transport – Part 2: Steady-state changes in ozone air quality and impacts on human mortality. Atmospheric Chemistry and Physics, 9(16), DOI:10.5194/acp-9-6095-2009. Abstract
Large-scale changes in ozone precursor emissions affect ozone directly in the short term, and also affect methane, which in turn causes long-term changes in ozone that affect surface ozone air quality. Here we assess the effects of changes in ozone precursor emissions on the long-term change in surface ozone via methane, as a function of the emission region, by modeling 10% reductions in anthropogenic nitrogen oxide (NOx) emissions from each of nine world regions. Reductions in NOx emissions from all world regions increase methane and long-term surface ozone. While this long-term increase is small compared to the intra-regional short-term ozone decrease, it is comparable to or larger than the short-term inter-continental ozone decrease for some source-receptor pairs. The increase in methane and long-term surface ozone per ton of NOx reduced is greatest in tropical and Southern Hemisphere regions, exceeding that from temperate Northern Hemisphere regions by roughly a factor of ten. We also assess changes in premature ozone-related human mortality associated with regional precursor reductions and long-range transport, showing that for 10% regional NOx reductions, the strongest inter-regional influence is for emissions from Europe affecting mortalities in Africa. Reductions of NOx in North America, Europe, the Former Soviet Union, and Australia are shown to reduce more mortalities outside of the source regions than within. Among world regions, NOx reductions in India cause the greatest number of avoided mortalities per ton, mainly in India itself. Finally, by increasing global methane, NOx reductions in one hemisphere tend to cause long-term increases in ozone concentration and mortalities in the opposite hemisphere. Reducing emissions of methane, and to a lesser extent carbon monoxide and non-methane volatile organic compounds, alongside NOx reductions would avoid this disbenefit.
Reducing methane (CH4) emissions is an attractive option for jointly addressing climate and ozone (O3) air quality goals. With multidecadal full-chemistry transient simulations in the MOZART-2 tropospheric chemistry model, we show that tropospheric O3 responds approximately linearly to changes in CH4 emissions over a range of anthropogenic emissions from 0–430 Tg CH4a−1 (0.11–0.16 Tg tropospheric O3 or ∼11–15 ppt global mean surface O3 decrease per Tg a−1 CH4 reduced). We find that neither the air quality nor climate benefits depend strongly on the location of the CH4 emission reductions, implying that the lowest cost emission controls can be targeted. With a series of future (2005–2030) transient simulations, we demonstrate that cost-effective CH4 controls would offset the positive climate forcing from CH4 and O3 that would otherwise occur (from increases in NOx and CH4 emissions in the baseline scenario) and improve O3 air quality. We estimate that anthropogenic CH4 contributes 0.7 Wm−2 to climate forcing and ∼4 ppb to surface O3 in 2030 under the baseline scenario. Although the response of surface O3 to CH4 is relatively uniform spatially compared to that from other O3 precursors, it is strongest in regions where surface air mixes frequently with the free troposphere and where the local O3 formation regime is NOx-saturated. In the model, CH4 oxidation within the boundary layer (below ∼2.5 km) contributes more to surface O3 than CH4 oxidation in the free troposphere. In NOx-saturated regions, the surface O3 sensitivity to CH4 can be twice that of the global mean, with >70% of this sensitivity resulting from boundary layer oxidation of CH4. Accurately representing the NOx distribution is thus crucial for quantifying the O3 sensitivity to CH4.
Biomass burning is a major source of air
pollutants, some of which are also climate forcing agents. We investigate
the sensitivity of direct radiative forcing due to tropospheric ozone and
aerosols (carbonaceous and sulfate) to a marginal reduction in their (or
their precursor) emissions from major biomass burning regions. We find that
the largest negative global forcing is for 10% emission reductions in
tropical regions, including Africa (−4.1 mWm−2 from gas and −4.1
mWm−2 from aerosols), and South America (−3.0 mWm−2
from gas and −2.8 mWm−2 from aerosols). We estimate that a unit
reduction in the amount of biomass burned in India produces the largest
negative ozone and aerosol forcing. Our analysis indicates that reducing
biomass burning emissions causes negative global radiative forcing due to
ozone and aerosols; however, regional differences need to be considered when
evaluating controls on biomass burning to mitigate global climate change.
Changes in emissions of ozone (O3) precursors affect both air
quality and climate. We first examine the sensitivity of surface O3
concentrations (O3srf) and net radiative forcing of
climate (RFnet) to reductions in emissions of four precursors -
nitrogen oxides (NOx), non-methane volatile organic
compounds, carbon monoxide, and methane (CH4). We show that
long-term CH4-induced changes in O3, known to be
important for climate, are also relevant for air quality; for example, NOxreductions increase CH4, causing a long-term O3
increase that partially counteracts the direct O3 decrease.
Second, we assess the radiative forcing resulting from actions to improve O3
air quality by calculating the ratio of ΔRFnet
to changes in metrics of O3srf. Decreases in CH4
emissions cause the greatest RFnet decrease per unit reduction
in O3srf, while NOxreductions
increase RFnet. Of the available means to improve O3
air quality, therefore, CH4 abatement best reduces climate
forcing.
The global distribution of tropospheric ozone (O3) depends on the emission of precursors, chemistry, and transport. For small perturbations to emissions, the global radiative forcing resulting from changes in O3 can be expressed as a sum of forcings from emission changes in different regions. Tropospheric O3 is considered in present climate policies only through the inclusion of indirect effect of CH4 on radiative forcing through its impact on O3 concentrations. The short-lived O3 precursors (NOx , CO, and NMHCs) are not directly included in the Kyoto Protocol or any similar climate mitigation agreement. In this study, we quantify the global radiative forcing resulting from a marginal reduction (10%) in anthropogenic emissions of NOx alone from nine geographic regions and a combined marginal reduction in NOx , CO, and NMHCs emissions from three regions. We simulate, using the global chemistry transport model MOZART-2, the change in the distribution of global O3 resulting from these emission reductions. In addition to the short-term reduction in O3, these emission reductions also increase CH4concentrations (by decreasing OH); this increase in CH4 in turn counteracts part of the initial reduction in O3 concentrations. We calculate the global radiative forcing resulting from the regional emission reductions, accounting for changes in both O3 and CH4. Our results show that changes in O3 production and resulting distribution depend strongly on the geographical location of the reduction in precursor emissions. We find that the global O3 distribution and radiative forcing are most sensitive to changes in precursor emissions from tropical regions and least sensitive to changes from midlatitude and high-latitude regions. Changes in CH4 and O3 concentrations resulting from NOx emission reductions alone produce offsetting changes in radiative forcing, leaving a small positive residual forcing (warming) for all regions. In contrast, for combined reductions of anthropogenic emissions of NOx , CO, and NMHCs, changes in O3 and CH4 concentrations result in a net negative radiative forcing (cooling). Thus we conclude that simultaneous reductions of CO, NMHCs, and NOx lead to a net reduction in radiative forcing due to resulting changes in tropospheric O3 and CH4 while reductions in NOx emissions alone do not.
