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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 ensemble 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, but there is a suggestion of a high bias in the Northern Hemisphere and a low bias in the Southern Hemisphere, which could indicate deficiencies with the ozone precursor emissions. Compared to the present day ensemble mean tropospheric ozone burden of 337 ± 23 Tg, the ensemble 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 in the ensemble mean tropospheric ozone burden in 2030 (2100) for the different RCPs are: −4% (−16%) for RCP2.6, 2% (−7%) for RCP4.5, 1% (−9%) for RCP6.0, and 7% (18%) for RCP8.5. Model agreement on the magnitude of the change is greatest for larger changes. Reductions in most precursor emissions are common across the RCPs and drive ozone decreases in all but RCP8.5, where doubled methane and a 40–150% greater stratospheric influx (estimated from a subset of models) increase ozone. While models with a high ozone burden for the present day also have high ozone burdens for the other time slices, no model consistently predicts large or small ozone changes; i.e. the magnitudes of the burdens and burden changes do not appear to be related simply, and the models are sensitive to emissions and climate changes in different ways. 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 and a rigorous investigation of the factors that drive tropospheric ozone is recommended to help future studies attribute ozone changes and inter-model differences more clearly.

Increases in surface ozone (O3) and fine particulate matter (≤2.5 μm aerodynamic diameter, PM2.5) are associated with excess premature human mortalities. We estimate changes in surface O3 and PM2.5 from pre-industrial (1860) to present (2000) and the global present-day (2000) premature human mortalities associated with these changes. We extend previous work to differentiate the contribution of changes in three factors: emissions of short-lived air pollutants, climate change, and increased methane (CH4) concentrations, to air pollution levels and 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 (results reported as annual average ±standard deviation of 10-yr model simulations), 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 population-weighted 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 0.04 ± 0.24 μg m−3 (+4.3 ± 0.33 ppbv), respectively. Total global changes in PM2.5 are associated with 1.5 (95% confidence interval, CI, 1.2–1.8) million cardiopulmonary mortalities and 95 (95% CI, 44–144) thousand lung cancer mortalities annually and changes 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 contribute to premature mortality associated with air pollution globally (by 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. Our study highlights the benefits to air quality and human health of CH4 mitigation as a component of future air pollution control policy.

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. Plain Language Summary GFDL has developed a coupled chemistry‐carbon‐climate Earth System Model (ESM4.1) as part of its fourth‐generation coupled model development activities with model results contributed publicly to the sixth phase of the Coupled Model Intercomparison Project. With similar computational expense as GFDL's first coupled model CM4.0, ESM4.1 focuses on chemistry and ecosystem comprehensiveness rather than the ocean resolution‐focus of CM4.0. With fidelity near to that of CM4.0, ESM4.1 features much improved representation of climate mean patterns and variability from previous GFDL ESMs as well as comprehensive couplings for chemistry, carbon, and dust. Key Points A new coupled chemistry‐carbon‐climate Earth system model has been developed at the Geophysical Fluid Dynamics Laboratory This model unifies component advances in chemistry, carbon, and ecosystem comprehensiveness within a single coupled climate framework This model features much improved climate mean patterns and variability from previous chemistry and carbon coupled models

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 Coupled 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 day−1. However, when using a version of CM3 with reduced present-day aerosol radiative forcing (−1.0 W m−2), the global temperature increase for RCP8.5 is about 0.5 K, with similar magnitude decreases in other climate response parameters as well. Regionally and locally, climate impacts can be much larger than the global mean, 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 day−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 (or 10–20 % with weaker aerosol forcing) 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.

We describe the Geophysical Fluid Dynamics Laboratory'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 preindustrial 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 quasiperiodicity 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. Plain Language Summary The Geophysical Fluid Dynamics Laboratory (GFDL) of the National Oceanic and Atmospheric Administration participates along with a number of model centers around the world in constructing state‐of‐the‐art climate models for use in studies for climate change and prediction. GFDL's latest multipurpose atmosphere‐ocean coupled climate model, CM4.0, is described here. It consists of GFDL's latest atmosphere and land models at about 100 km horizontal resolution and ocean and sea ice models at roughly 25 km horizontal resolution. A handful of standard experiments have been conducted with CM4.0 for participation in the Coupled Model Intercomparison Project Phase 6, an archive of climate model results utilized by the Intergovernmental Panel on Climate Change and the climate research community more generally. The model results have been extensively evaluated against observations. This paper makes the case that CM4.0 ranks high among state‐of‐the‐art coupled climate models by many measures of bias in the simulated climatology and in its ability to capture modes of climate variability such as the El Niño‐Southern Oscillation and Madden‐Julian Oscillation. The paper also discusses some potential weaknesses, including unrealistically large internal variability in the Southern Ocean and insufficient warming before 1990 in the simulation of the twentieth century. Key Points A team at GFDL has developed a new model of the physical climate system referred to as CM4.0 Strengths of model include ENSO simulation and small biases in TOA fluxes, precipitation, Arctic sea ice extent, and sea surface temperature Problematic aspects include large variability in Southern Ocean and historical simulation with little warming prior to 1990

We have analysed time-slice simulations from 17 global models, participating in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), to explore changes in present-day (2000) hydroxyl radical (OH) concentration and methane (CH4) lifetime relative to preindustrial times (1850) and to 1980. A comparison of modeled and observation-derived methane and methyl chloroform lifetimes suggests that the present-day global multimodel mean OH concentration is overestimated by 5 to 10% but is within the range of uncertainties. The models consistently simulate higher OH concentrations in the Northern Hemisphere (NH) compared with the Southern Hemisphere (SH) for the present-day (2000; inter-hemispheric ratios of 1.13 to 1.42), in contrast to observation-based approaches which generally indicate higher OH in the SH although uncertainties are large. Evaluation of simulated carbon monoxide (CO) concentrations, the primary sink for OH, against ground-based and satellite observations suggests low biases in the NH that may contribute to the high north–south OH asymmetry in the models. The models vary widely in their regional distribution of present-day OH concentrations (up to 34 %). Despite large regional changes, the multi-model global mean (mass-weighted) OH concentration changes little over the past 150 yr, due to concurrent increases in factors that enhance OH (humidity, tropospheric ozone, nitrogen oxide (NOx) emissions, and UV radiation due to decreases in stratospheric ozone), compensated by increases in OH sinks (methane abundance, carbon monoxide and non-methane volatile organic carbon (NMVOC) emissions). The large inter-model diversity in the sign and magnitude of preindustrial to present-day OH changes (ranging from a decrease of 12.7% to an increase of 14.6 %) indicate that uncertainty remains in our understanding of the long-term trends in OH and methane lifetime. We show that this diversity is largely explained by the different ratio of the change in global mean tropospheric CO and NOx burdens (1CO/1NOx, approximately represents changes in OH sinks versus changes in OH sources) in the models, pointing to a need for better constraints on natural precursor emissions and on the chemical mechanisms in the current generation of chemistry-climate models. For the 1980 to 2000 period, we find that climate warming and a slight increase in mean OH (3.5±2.2 %) leads to a 4.3±1.9% decrease in the methane lifetime. Analysing sensitivity simulations performed by 10 models, we find that preindustrial to presentday climate change decreased the methane lifetime by about four months, representing a negative feedback on the climate system. Further, we analysed attribution experiments performed by a subset of models relative to 2000 conditions with only one precursor at a time set to 1860 levels. 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.

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 (9.3+/-0.9 yr when only including selected models), 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 RCP8.5. 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 OH was found to be associated more strongly with differences in modelled temperature and stratospheric ozone changes. Finally, through perturbation experiments we calculated an OH feedback factor (F) of 1.24 from present day conditions (1.50 from 2100 RCP8.5 conditions) and a climate feedback on methane lifetime of 0.33+-0.13 yr/K, on average. Models that did not include interactive stratospheric ozone effects on photolysis showed a stronger sensitivity to climate, as they did not account for negative effects of climate-driven stratospheric ozone recovery on tropospheric OH, which would have partly offset the overall OH/methane lifetime response to climate change.

The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) consists of a series of time slice experiments targeting the long-term changes in atmospheric composition between 1850 and 2100, with the goal of documenting composition changes and the associated radiative forcing. In this overview paper, we introduce the ACCMIP activity, the various simulations performed (with a requested set of 14) and the associated model output. The 16 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 are responsible for a significant range across models, mostly in the case of 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. However, models that are clear outliers are different enough from the other models to significantly affect their simulation of atmospheric chemistry.

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 fine nitrate optical depth at 550 nm in 2010 is 0.006 (0.005–0.008). In wintertime, nitrate aerosols are simulated to account for over 30 % of the aerosol optical depth over western Europe and North America. Simulated nitrate optical depth increases by less than 30 % (0.0061–0.010) in response to projected changes in anthropogenic emissions from 2010 to 2050 (e.g., −40 % for SO2 and +38 % for ammonia). This increase is primarily driven by greater concentrations of nitrate in the free troposphere, while surface nitrate concentrations decrease in the midlatitudes following lower concentrations of nitric acid. With the projected increase of ammonia emissions, we show that better constraints on the vertical distribution of ammonia (e.g., convective transport and biomass burning injection) and on the sources and sinks of nitric acid (e.g., heterogeneous reaction on dust) are needed to improve estimates of future nitrate optical depth.

Understanding the surface O3 response over a “receptor” region to emission changes over a foreign “source” region is key to evaluating the potential gains from an international approach to abate ozone (O3) pollution. We apply an ensemble of 21 global and hemispheric chemical transport models to estimate the spatial average surface O3 response over east Asia (EA), Europe (EU), North America (NA), and south Asia (SA) to 20% decreases in anthropogenic emissions of the O3 precursors, NOx, NMVOC, and CO (individually and combined), from each of these regions. We find that the ensemble mean surface O3 concentrations in the base case (year 2001) simulation matches available observations throughout the year over EU but overestimates them by >10 ppb during summer and early fall over the eastern United States and Japan. The sum of the O3 responses to NOx, CO, and NMVOC decreases separately is approximately equal to that from a simultaneous reduction of all precursors. We define a continental‐scale “import sensitivity” as the ratio of the O3 response to the 20% reductions in foreign versus “domestic” (i.e., over the source region itself) emissions. For example, the combined reduction of emissions from the three foreign regions produces an ensemble spatial mean decrease of 0.6 ppb over EU (0.4 ppb from NA), less than the 0.8 ppb from the reduction of EU emissions, leading to an import sensitivity ratio of 0.7. The ensemble mean surface O3 response to foreign emissions is largest in spring and late fall (0.7–0.9 ppb decrease in all regions from the combined precursor reductions in the three foreign regions), with import sensitivities ranging from 0.5 to 1.1 (responses to domestic emission reductions are 0.8–1.6 ppb). High O3 values are much more sensitive to domestic emissions than to foreign emissions, as indicated by lower import sensitivities of 0.2 to 0.3 during July in EA, EU, and NA when O3 levels are typically highest and by the weaker relative response of annual incidences of daily maximum 8‐h average O3 above 60 ppb to emission reductions in a foreign region (<10–20% of that to domestic) as compared to the annual mean response (up to 50% of that to domestic). Applying the ensemble annual mean results to changes in anthropogenic emissions from 1996 to 2002, we estimate a Northern Hemispheric increase in background surface O3 of about 0.1 ppb a−1, at the low end of the 0.1–0.5 ppb a−1 derived from observations. From an additional simulation in which global atmospheric methane was reduced, we infer that 20% reductions in anthropogenic methane emissions from a foreign source region would yield an O3 response in a receptor region that roughly equals that produced by combined 20% reductions of anthropogenic NOx, NMVOC, and CO emissions from the foreign source region.