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At least 19 records

Comparison of Arctic and Antarctic Stratospheric Climates in Chemistry Versus No‐Chemistry Climate Models

Using nine chemistry-climate and eight associated no-chemistry models, we investigate the persistence and timing of cold episodes occurring in the Arctic and Antarctic stratosphere during the period 1980–2014. We find systematic differences in behavior between members of these model pairs. In a first group of chemistry models whose dynamical configurations mirror their no-chemistry counterparts, we find an increased persistence of such cold polar vortices, such that these cold episodes often start earlier and last longer, relative to the times of occurrence of the lowest temperatures. Also the date of occurrence of the lowest temperatures, both in the Arctic and the Antarctic, is often delayed by 1–3 weeks in chemistry models, versus their no-chemistry counterparts. This behavior exacerbates a widespread problem occurring in most or all models, a delayed occurrence, in the median, of the most anomalously cold day during such cold winters. In a second group of model pairs there are differences beyond just ozone chemistry. In particular, here the chemistry models feature more levels in the stratosphere, a raised model top, and differences in non-orographic gravity wave drag versus their no-chemistry counterparts. Such additional dynamical differences can completely mask the above influence of ozone chemistry. The results point toward a need to retune chemistry-climate models versus their no-chemistry counterparts.

54 ENVIRONMENTAL SCIENCES↗

Machine learning-based bias-corrected future projections of ozone concentrations from a chemistry-climate model

Reliable projection of future near-surface ozone is crucial for air quality management and health risk assessment. However, potential biases in spatial distribution, magnitude and trends in ozone concentrations simulated by global chemistry-climate models limit their applicability in regional-scale evaluations. In this study, LightGBM, a machine learning (ML) algorithm is applied to correct biases in CESM2-simulated ozone concentrations over China, the United States and Europe and calibrate future ozone projections under two diverse Shared Socioeconomic Pathways (SSP1-2.6 and SSP5-8.5) scenarios from 2020 to 2060. The ML-based correction significantly improves the spatial distribution and reduces the model bias by 40%–60%. It also reverses the potentially incorrect trend of ozone change under SSP1-2.6 in eastern China. When applying ML-based bias correction to CESM2 future projections, warm season mean ozone concentrations decrease across China, the United States, and Europe by –13.5, –17.9, and –13.7 µg/m³, respectively, between 2020 and 2060 in SSP1-2.6, while they increase by 9.4, 2.0, and 5.2 µg/m³ in SSP5-8.5. Decomposition analysis show that changes in anthropogenic emissions dominate future ozone changes in both scenarios, while strong climate penalty from ozone changes occurs in polluted eastern China and climate benefit is found in western China, the United States and Europe under SSP5-8.5. These findings demonstrate the value of combining ML with chemistry-climate models to produce more accurate air quality projections, thereby informing more effective and region-specific environmental protection strategies.

Chemistry Model↗

The GFDL Variable-Resolution Global Chemistry-Climate Model for Research at the Nexus of US Climate and Air Quality Extremes

We present a variable-resolution global chemistry-climate model (AM4VR) developed at NOAA's Geophysical Fluid Dynamics Laboratory (GFDL) for research at the nexus of US climate and air quality extremes. AM4VR has a horizontal resolution of 13 km over the US, allowing it to resolve urban-to-rural chemical regimes, mesoscale convective systems, and land-surface heterogeneity. With the resolution gradually reducing to 100 km over the Indian Ocean, we achieve multi-decadal simulations driven by observed sea surface temperatures at 50% of the computational cost for a 25-km uniform-resolution grid. In contrast with GFDL's AM4.1 contributing to the sixth Coupled Model Intercomparison Project at 100 km resolution, AM4VR features much improved US climate mean patterns and variability. In particular, AM4VR shows improved representation of: precipitation seasonal-to-diurnal cycles and extremes, notably reducing the central US dry-and-warm bias; western US snowpack and summer drought, with implications for wildfires; and the North American monsoon, affecting dust storms. AM4VR exhibits excellent representation of winter precipitation, summer drought, and air pollution meteorology in California with complex terrain, enabling skillful prediction of both extreme summer ozone pollution and winter haze events in the Central Valley. AM4VR also provides vast improvements in the process-level representations of biogenic volatile organic compound emissions, interactive dust emissions from land, and removal of air pollutants by terrestrial ecosystems. We highlight the value of increased model resolution in representing climate–air quality interactions through land-biosphere feedbacks. AM4VR offers a novel opportunity to study global dimensions to US air quality, especially the role of Earth system feedbacks in a changing climate.

54 ENVIRONMENTAL SCIENCES↗

Implementing and Improving CBMZ-MAM3 Chemistry and Aerosol Modules in the Regional Climate Model WRF-CAM5: An Evaluation over the Western US and Eastern North Pacific

The representation of aerosols in climate-chemistry models is important for air quality and climate change research, but it can require significant computational resources. The objective of this study was to improve the representation of aerosols in climate–chemistry models, specifically in the carbon bond mechanism, version Z (CBMZ), and modal aerosol modules with three lognormal modes (MAM3) in the WRF-CAM5 model. The study aimed to enhance the model’s chemistry capabilities by incorporating biomass burning emissions, establishing a conversion mechanism between volatile organic compounds (VOCs) and secondary organic carbons (SOCs), and evaluating its performance against observational benchmarks. The results of the study demonstrated the effectiveness of the enhanced chemistry capabilities in the WRF-CAM5 model. Six simulations were conducted over the western U.S. and northeastern Pacific region, comparing the model’s performance with observational benchmarks such as reanalysis, ground-based, and satellite data. The findings revealed a significant reduction in root-mean-square errors (RMSE) for surface concentrations of black carbon (BC) and organic carbon (OC). Specifically, the model exhibited a 31% reduction in RMSE for BC concentrations and a 58% reduction in RMSE for OC concentrations. These outcomes underscored the importance of accurate aerosol representation in climate-chemistry models and emphasized the potential for improving simulation accuracy and reducing errors through the incorporation of enhanced chemistry modules in such models.

54 ENVIRONMENTAL SCIENCES↗

Hunga Tonga–Hunga Ha′apai Volcano Impact Model Observation Comparison (HTHH-MOC) project: experiment protocol and model descriptions

The 2022 Hunga volcanic eruption injected a significant amount of water vapor and a moderate amount of sulfur dioxide into the stratosphere, causing observable responses in the climate system. We have developed a model–observation comparison project to investigate the evolution of volcanic water and aerosols and their impacts on atmospheric dynamics, chemistry, and climate, using several state-of-the-art chemistry climate models. The project goals are (1) to evaluate the current chemistry–climate models to quantify their performance in comparison to observations and (2) to understand atmospheric responses in the Earth system after this exceptional event and investigate the potential impacts in the projected future. To achieve these goals, we designed specific experiments for direct comparisons to observations, for example from balloons and the Microwave Limb Sounder satellite instrument. Experiment 1 consists of two sets of free-running ensemble experiments from 2022 to 2031: one with fixed sea-surface temperatures and sea ice and one with coupled ocean. These experiments will help to understand the long-term evolution of water vapor and aerosols; quantify HTHH effects on stratospheric and mesospheric temperatures, dynamics, and transport; understand the impact of dynamic changes on ozone chemistry; quantify the net radiative forcings; and evaluate any surface climate impact. Experiment 2 is a nudged-run experiment from 2022 to 2023 using observed meteorology. To allow participation of more climate models with varying complexities of aerosol simulation, we include two sets of simulations in Experiment 2: Experiment 2a is designed for models with internally generated aerosol, while Experiment 2b is designed for models using prescribed aerosol surface area density. This experiment will help to analyze H 2 O and aerosol evolution, quantify the net radiative forcings, understand the impacts on mid-latitude and polar O 3 chemistry, and allow close comparisons with observations.

Zhu, Yunqian [Univ. of Colorado, Boulder, CO (Unit↗

An inconsistency in aviation emissions between CMIP5 and CMIP6 and the implications for short-lived species and their radiative forcing

We report on an inconsistency in the latitudinal distribution of aviation emissions between the data products of phases 5 and 6 of the Coupled Model Intercomparison Project (CMIP). Emissions in the CMIP6 data occur at higher latitudes than in the CMIP5 data for all scenarios, years, and emitted species. A comparative simulation with the chemistry–climate model ECHAM/MESSy Atmospheric Chemistry (EMAC) reveals that the difference in nitrogen oxide emission distribution leads to reduced overall ozone changes due to aviation in the CMIP6 scenarios because in those scenarios the distribution of emissions is partly shifted towards the chemically less active higher latitudes. The radiative forcing associated with aviation ozone is 7.6 % higher, and the decrease in methane lifetime is 5.7 % larger for the year 2015 when using the CMIP5 latitudinal distribution of emissions compared to when using the CMIP6 distribution. We do not find a statistically significant difference in the radiative forcing associated with aviation aerosol emissions. In total, future studies investigating the effects of aviation emissions on ozone and climate should consider the inconsistency reported here.

54 ENVIRONMENTAL SCIENCES↗

Development and Evaluation of Chemistry‐Aerosol‐Climate Model CAM5‐Chem‐MAM7‐MOSAIC: Global Atmospheric Distribution and Radiative Effects of Nitrate Aerosol

Abstract An advanced aerosol treatment, with a focus on semivolatile nitrate formation, is introduced into the Community Atmosphere Model version 5 with interactive chemistry (CAM5‐chem) by coupling the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) with the 7‐mode Modal Aerosol Module (MAM7). An important feature of MOSAIC is dynamic partitioning of all condensable gases to the different fine and coarse mode aerosols, as governed by mode‐resolved thermodynamics and heterogeneous chemical reactions. Applied in the free‐running mode from 1995 to 2005 with prescribed historical climatological conditions, the model simulates global distributions of sulfate, nitrate, and ammonium in good agreement with observations and previous studies. Inclusion of nitrate resulted in ∼10% higher global average accumulation mode number concentrations, indicating enhanced growth of Aitken mode aerosols from nitrate formation. While the simulated accumulation mode nitrate burdens are high over the anthropogenic source regions, the sea‐salt and dust modes respectively constitute about 74% and 17% of the annual global average nitrate burden. Regional clear‐sky shortwave radiative cooling of up to −5 W m −2 due to nitrate is seen, with a much smaller global average cooling of −0.05 W m −2 . Significant enhancements in regional cloud condensation nuclei (at 0.1% supersaturation) and cloud droplet number concentrations are also attributed to nitrate, causing an additional global average shortwave cooling of −0.8 W m −2 . Taking into consideration of changes in both longwave and shortwave radiation under all‐sky conditions, the net change in the top of the atmosphere radiative fluxes induced by including nitrate aerosol is −0.7 W m −2 .

54 ENVIRONMENTAL SCIENCES↗

Implementation of Sub‐Grid Scale Temperature Perturbations Induced by Non‐Orographic Gravity Waves in WACCM6

Abstract Atmospheric gravity waves can play a significant role on atmospheric chemistry through temperature fluctuations. A recent modeling study introduced a method to implement subgrid‐scale orographic gravity‐wave‐induced temperature perturbations in the Whole Atmosphere Community Climate Model (WACCM). The model with a wave‐induced temperature parameterization was able to reproduce for example, the influence of mountain wave events on atmospheric chemistry, as highlighted in previous literature. Here we extend the subgrid‐scale wave‐induced temperature parameterization to also include non‐orographic gravity waves arising from frontal activity and convection. We explore the impact of these waves on middle atmosphere chemistry, particularly focusing on reactions that are strongly sensitive to temperature. The non‐orographic gravity waves increase the variability of chemical reaction rates, especially in the lower mesosphere. As an example, we show that this, in turn, leads to increases in the daytime ozone variability. To demonstrate another impact, we briefly investigate the role of non‐orographic gravity waves in cirrus cloud formation in this model. Consistent with findings from the previous study focusing on orographic gravity waves, non‐orographic waves also enhance homogeneous nucleation and increase cirrus clouds. The updated method used enables the global chemistry‐climate model to account for both orographic and non‐orographic gravity‐wave‐induced subgrid‐scale dynamical perturbations in a consistent manner.

Yook, Simchan [Department of Earth Atmospheric and↗

Studying Cloud and Radiative Impacts Through an Improved Physically Based Representation of Organic Aerosol in a Large-Scale Model (WRF-Chem) (Final Report)

The work performed under this award resulted in the development of a computationally-efficient kinetic model to simulate the chemistry, thermodynamics, and microphysics of organic aerosol. Versions of the kinetic model were used to study a suite of aerosol processes including, multigenerational gas-phase chemistry, phase-state influenced gas/particle partitioning, heterogeneous oxidation, oligomerization reactions, and experimental artifacts. The kinetic model has now been implemented into a regional chemistry-climate model (WRF-Chem) to further study the formation, evolution, properties, and spatiotemporal distribution of organic aerosol at urban, regional, and global scales.

54 ENVIRONMENTAL SCIENCES↗

Validating a microphysical prognostic stratospheric aerosol implementation in E3SMv2 using observations after the Mount Pinatubo eruption

Abstract. This paper describes the addition of a stratospheric prognostic aerosol (SPA) capability – developed with the goal of accurately simulating sulfate aerosol formation and evolution in the stratosphere – in the Department of Energy (DOE) Energy Exascale Earth System Model, version 2 (E3SMv2). The implementation includes changes to the four-mode Modal Aerosol Module microphysics in the stratosphere to allow for larger particle growth and more accurate stratospheric aerosol lifetime following the Pinatubo eruption. E3SMv2-SPA reasonably reproduces stratospheric aerosol lifetime, burden, aerosol optical depth, and top-of-atmosphere flux when compared to remote sensing observations. E3SMv2-SPA also has close agreement with the interactive chemistry–climate model CESM2-WACCM (Community Earth System Model version 2–Whole Atmosphere Community Climate Model) – which has a more complete chemical treatment – and the observationally constrained, prescribed volcanic aerosol treatment in E3SMv2. Global stratospheric aerosol size distributions identify the nucleation and growth of sulfate aerosol from volcanically injected SO2 from both major and minor volcanic eruptions from 1991 to 1993. The modeled aerosol effective radius is consistently lower than satellite and in situ measurements (max differences of ∼ 30 %). Comparisons with in situ size distribution samples indicate that this simulated underestimation in both E3SMv2-SPA and CESM2-WACCM is due to overly small accumulation and coarse-mode aerosols 6–18 months post-eruption, with E3SMv2-SPA simulating ∼ 50 % of the coarse-mode geometric mean diameters of observations 11 months post-eruption. Effective radii from the models and observations are used to calculate offline scattering and absorption efficiencies to explore the implications of smaller simulated aerosol size for the Pinatubo climate impacts. Scattering efficiencies at wavelengths of peak solar irradiance (∼ 0.5 µm) are 10 %–80 % higher for daily samples in models relative to observations through 1993, suggesting higher diffuse radiation at the surface and a larger cooling effect in the models due to the smaller simulated aerosol; absorption efficiencies at the peak wavelengths of outgoing terrestrial radiation (∼ 10 µm) are 15 %–40 % lower for daily samples in models relative to observations, suggesting an underestimation in stratospheric heating in the models due to the smaller simulated aerosol. These potential biases are based on aerosol size alone and do not take into account differences in the aerosol number. The overall agreement of E3SMv2-SPA with observations and its similar performance to the well-validated CESM2-WACCM makes E3SMv2-SPA a viable alternative to simulating climate impacts from stratospheric sulfate aerosols.

Brown, Hunter York (ORCID:0000000218147874)↗

Comparing the Effect of Anthropogenically Amplified Halogen Natural Emissions on Tropospheric Ozone Chemistry Between Pre-Industrial and Present-Day

Reactive halogens (X + XO, X = I, Br or Cl) catalytically destroy a fraction of tropospheric ozone under present-day (PD) conditions, however, their distribution and potential impact on tropospheric ozone under pre-industrial (PI) conditions remain largely unexplored. This study uses the Community Atmosphere Model with Chemistry (CAM-Chem) to investigate the effect of anthropogenically amplified natural emissions of halogenated species and their subsequent chemistry on tropospheric ozone under PI and PD atmospheric conditions. Model results show that the global tropospheric ozone depletion due to natural halogens is slightly more sensitive in PI than PD, with percentage changes in tropospheric ozone burden (TOB) of -14.1 ± 0.6% for PI and -12.9 ± 0.6% for PD. Individually, the role of iodine and chlorine in ozone depletion is equivalent in both periods (ΔTOB I : ~-7% and ΔTOB Cl : ~-2.5%), while bromine plays a larger role in PI (ΔTOB Br : -5.5 ± 0.6%) versus PD (ΔTOB Br : -4.3 ± 0.7%). The increase in anthropogenic ozone precursor emissions from PI to PD has amplified the natural emission of inorganic halogens and led to a shift in the partitioning of inorganic halogens from reactive to reservoir species. Consequently, halogen-driven ozone depletion from the surface to the free troposphere is larger in PI than PD. In contrast, in the upper troposphere, the ozone depletion is larger in PD influenced mainly by stratospheric intrusion of reactive halogens from long-lived species. This study highlights the importance of including a complete chemical coupling of natural halogens and atmospheric pollutants in chemistry-climate models to adequately assess their effects on tropospheric ozone in a changing climate.

54 ENVIRONMENTAL SCIENCES↗

Source attribution of near-surface ozone trends in the United States during 1995–2019

Emissions of ozone (O 3 ) precursors in the United States have decreased in recent decades, and near-surface O 3 concentrations showed a significant decrease in summer but an increase in winter. In this study, an O 3 source tagging technique is utilized in a chemistry–climate model to investigate the source contributions to O 3 mixing ratios in the US from various emitting sectors and regions of nitrogen oxides (NO x ) and reactive carbon species during 1995–2019. We show that domestic emission reductions from energy and surface transportation are primarily responsible for the decrease in summertime O 3 during 1995–2019. However, in winter, the emission control also weakens the NO x titration process, resulting in considerable increases in O 3 levels from natural sources. Additionally, increases in aviation and shipping emissions and transpacific transport of O 3 from Asia largely contribute to the winter O 3 increase. We also found that changes in large-scale circulation favoring O 3 transport from the upper atmosphere and foreign transport from Asia also explain 15 % of the increase in the US near-surface O 3 levels in winter.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Source attribution of near-surface ozone pollution in Jiangsu Province of China over 2013–2019

Near-surface ozone (O3) is one of the most severe air pollutants in China, particularly over densely populated Jiangsu Province in the Yangtze River Delta. In this study, an O3 source tagging technique is utilized in a chemistry-climate model to quantify the source contributions of various emission sectors and regions for nitrogen oxides (NOx) and volatile organic compounds (VOCs) to O3 concentrations in Jiangsu Province during 2013–2019. The results show that the near-surface O3 in Jiangsu Province is mainly contributed by surrounding and remote anthropogenic NOx emissions through long-range transport. Local anthropogenic NOx emissions account for only 13 % and 18 % of the annual and summertime mean near-surface O3 in Jiangsu Province, respectively. Anthropogenic NOx emissions from the surface transportation, industry, and energy sectors account for 21 %, 22 % and 20 % of the annual mean near-surface O3 concentration in Jiangsu Province, respectively. Biogenic and anthropogenic VOCs emissions each explains one-third of the annual mean near-surface O3 concentration in Jiangsu, while methane and stratospheric chemical production contribute 21 % and 6 %, respectively. The sources from stratospheric production, aircraft, lightning, and foreign emissions are the primary contributors to O3 in the mid- and high troposphere. During high pollution days in Jiangsu Province, the near-surface O3 concentrations increase with the maximum exceeding 20 ppb, which is attributed to both the enhanced photochemical production and regional transport in favorable meteorological conditions.

ozone pollution↗

Rapid increase in tropospheric ozone over Southeast Asia attributed to changes in precursor emission source regions and sectors

Observations indicate that tropospheric ozone (O 3 ) concentrations over Southeast Asia have been increasing rapidly since the 1990s. Here, we quantify source contributions from geographical regions and emission sectors of the two distinct types of O 3 precursors, i.e., nitrogen oxides (NO x ) and volatile organic compounds (VOCs), to the increase in tropospheric O 3 in Southeast Asia during 1990–2019 using an O 3 source tagging technique implemented in a global chemistry-climate model. In this work, the results show that although local anthropogenic emission of NO x in Southeast Asia only contributes 18% of the annual averaged near-surface O 3 concentration, the increase in local NO x emission dominates the increasing trend of O 3 concentration in Southeast Asia, accounting for 107% of the regional averaged trend of 1.07 ppb decade -1 . Increases in NO x emissions from East Asia and South Asia explain 29% of the increasing trend, but 9% is offset by the emission reduction in North America. Ground transportation is responsible for 79% of the rapid O 3 increase, followed by 39% contribution from international shipping. Because an increase in anthropogenic NO x emissions enhances the O 3 production efficiency by VOCs, the increase in near-surface O 3 concentrations in Southeast Asia is thereby largely contributed by methane and biogenic VOCs.

54 ENVIRONMENTAL SCIENCES↗

Stratospheric Climate Anomalies and Ozone Loss Caused by the Hunga Tonga-Hunga Ha'apai Volcanic Eruption

We report the Hunga Tonga-Hunga Ha'apai (HTHH) volcanic eruption in January 2022 injected unprecedented amounts of water vapor (H 2 O) and a moderate amount of the aerosol precursor sulfur dioxide (SO 2 ) into the Southern Hemisphere (SH) tropical stratosphere. The H 2 O and aerosol perturbations have persisted during 2022 and early 2023 and dispersed throughout the atmosphere. Observations show large-scale SH stratospheric cooling, equatorward shift of the Antarctic polar vortex and slowing of the Brewer-Dobson circulation. Satellite observations show substantial ozone reductions over SH winter midlatitudes that coincide with the largest circulation anomalies. Chemistry-climate model simulations forced by realistic HTHH inputs of H 2 O and SO 2 qualitatively reproduce the observed evolution of the H 2 O and aerosol plumes over the first year, and the model exhibits stratospheric cooling, circulation changes and ozone effects similar to observed behavior. The agreement demonstrates that the observed stratospheric changes are caused by the HTHH volcanic influences.

58 GEOSCIENCES↗

Detecting tropospheric composition and climate responses to US air pollution controls in the context of internally-arising variability

Since the 1970s, air pollutant emissions controls in the United States (US) have lowered concentrations of ozone (O 3 ) and aerosols, which have opposing radiative effects on surface temperature. Using a pair of initial-condition ensembles generated by a fully-coupled chemistry-climate model, we simulate the “world avoided” by US air pollution controls. In this counterfactual world, we find tropospheric column O 3 increases, robust to natural internal variability, extending across the Northern Hemisphere. Robust aerosol increases, dominated by sulfate, remain localized near the US. Wintertime Northwest Atlantic cloud droplet number concentration is particularly sensitive to US aerosol. While an ensemble mean US surface cooling signal (−0.4 °C) implies that aerosol-driven cooling prevails over any O 3 -induced warming, we find that large regional internal variability will confound its detection in any single transient realization. Larger signal-to-noise ratios for composition versus climate variables underscore the greater detectability of emissions-driven changes in tropospheric composition compared to their associated climate impacts.

54 ENVIRONMENTAL SCIENCES↗

The Hunga Volcanic Eruption Atmospheric Impacts Report

On 15 January 2022 a highly explosive eruption of the Hunga volcano occurred in the Kingdom of Tonga in the South Pacific Ocean (175°24’ W, 20°33’ S). The Volcanic Explosivity Index (VEI) 6 eruption originated from a shallow submarine vent, making it distinct from large subaerial eruptions of recent decades (e.g., 1982 El Chichón, 1991 Mt. Pinatubo). In particular, seawater enhanced explosivity and dampened sulfur dioxide (SO 2 ) emissions. The eruption was the culmination of ~1 month of precursory activity; however, the timing and size of the eruption were unexpected, partly due to the challenges of monitoring submarine volcanoes. The stratospheric hydration caused by the eruption was unprecedented in magnitude, altitude, and duration in the satellite record. This Executive Summary reflects the current assessment of the Hunga eruption and its impact on the climate system. We report key observations of the eruption and its aftermath, as well as simulations of its impact by global chemistry-climate models. The Hunga eruption had an unprecedented impact on the stratosphere and mesosphere due to the plume height and large water content, which increased the global stratospheric water vapour burden by 10%. Most of this water has remained in the atmosphere into 2025. However, Hunga’s net impact on surface climate was small compared to that of earlier large-magnitude volcanic eruptions, due to limited sulfate aerosol loading in the stratosphere and the high altitude of the water vapour injection.

58 GEOSCIENCES↗

An approach to sulfate geoengineering with surface emissions of carbonyl sulfide

Sulfate geoengineering (SG) methods based on lower stratospheric tropical injection of sulfur dioxide (SO 2 ) have been widely discussed in recent years, focusing on the direct and indirect effects they would have on the climate system. Here a potential alternative method is discussed, where sulfur emissions are located at the surface or in the troposphere in the form of carbonyl sulfide (COS) gas. There are two time-dependent chemistry–climate model experiments designed from the years 2021 to 2055, assuming a 40 Tg-Syr -1 artificial global flux of COS, which is geographically distributed following the present-day anthropogenic COS surface emissions (SG-COS-SRF) or a 6 Tg-Syr -1 injection of COS in the tropical upper troposphere (SG-COS-TTL). The budget of COS and sulfur species is discussed, as are the effects of both SG-COS strategies on the stratospheric sulfate aerosol optical depth (~Δτ=0.080 in the years 2046–2055), aerosol effective radius (0.46 µm), surface SO x deposition (+8.9 % for SG-COS-SRF; +3.3 % for SG-COS-TTL), and tropopause radiative forcing (RF; ~-1.5 W m –2 in all-sky conditions in both SG-COS experiments). Indirect effects on ozone, methane and stratospheric water vapour are also considered, along with the COS direct contribution. According to our model results, the resulting net RF is –1.3 W m –2 , for SG-COS-SRF, and –1.5 W m –2 , for SG-COS-TTL, and it is comparable to the corresponding RF of –1.7 W m –2 obtained with a sustained injection of 4 Tg-Syr -1 in the tropical lower stratosphere in the form of SO 2 (SG-SO2, which is able to produce a comparable increase of the sulfate aerosol optical depth). Significant changes in the stratospheric ozone response are found in both SG-COS experiments with respect to SG-SO2 (~5 DU versus +1.4 DU globally). According to the model results, the resulting ultraviolet B (UVB) perturbation at the surface accounts for –4.3 % as a global and annual average (versus –2.4 % in the SG-SO2 case), with a springtime Antarctic decrease of –2.7 % (versus a +5.8 % increase in the SG-SO2 experiment). Overall, we find that an increase in COS emissions may be feasible and produce a more latitudinally uniform forcing without the need for the deployment of stratospheric aircraft. However, our assumption that the rate of COS uptake by soils and plants does not vary with increasing COS concentrations will need to be investigated in future work, and more studies are needed on the prolonged exposure effects to higher COS values in humans and ecosystems.

54 ENVIRONMENTAL SCIENCES↗