Amplified drying in South Asian summer monsoon precipitation due to anthropogenic sulfate aerosols.

A declining trend in Indian summer monsoon precipitation (ISMP) in the latter half of the 20th century is a scientifically challenging and societally relevant research issue. Heavy aerosol loading over India is one of the key factors in modulating the ISMP. Using the state-of-the-state-of-the-art chemistry-climate model, ECHAM6-HAMMOZ, the impacts of South Asian anthropogenic sulfate aerosols on the Indian summer monsoon precipitation were investigated against: (1) 2010 La Niña (excess monsoon), (2) 2015 El Niño (deficit monsoon) in comparison to (3) normal monsoon 2016. Sensitivity simulations were designed with 48% enhancement in South Asian SO2 emissions based on a trend estimated from Ozone Monitoring Instrument (OMI) satellite observations during 2006-2017. The model simulations showed that sulfate aerosols reduce ISMP by 27.5%-43.3 %, while simulations without sulfate loading enhanced ISMP by 23% in 2010 La Niña and reduction by 35% in 2015 El Niño. This paper reports that sulfate aerosols loading over India reduce precipitation by aerosol-induced direct and indirect effects by inducing atmospheric cooling, weakening in the convection, and reduction in moisture transport to Indian landmass. This paper emphasizes the necessity of alternate use of energy to reduce sulfate aerosol emissions to solve water issues in South Asia.

Optimal climate intervention scenarios for crop production vary by nation.

Stratospheric aerosol intervention (SAI) is a proposed strategy to reduce the effects of anthropogenic climate change. There are many temperature targets that could be chosen for a SAI implementation, which would regionally modify climatically relevant variables such as surface temperature, precipitation, humidity, total solar radiation and diffuse radiation. In this work, we analyse impacts on national maize, rice, soybean and wheat production by looking at output from 11 different SAI scenarios carried out with a fully coupled Earth system model coupled to a crop model. Higher-latitude nations tend to produce the most calories under unabated climate change, while midlatitude nations maximize calories under moderate SAI implementation and equatorial nations produce the most calories from crops under high levels of SAI. Our results highlight the challenges in defining 'globally optimal' SAI strategies, even if such definitions are based on just one metric.

Global Health and Climate Effects of Organic Aerosols from Different Sources.

The impact of aerosols on human health and climate is well-recognized, yet many studies have only focused on total PM2.5 or changes from anthropogenic activities. This study quantifies the health and climate effects of organic aerosols (OA) from anthropogenic, biomass burning, and biogenic sources. Using two atmospheric chemistry models, CAM-chem and GEOS-Chem, our findings reveal that anthropogenic primary OA (POA) has the highest efficiency for health effects but the lowest for direct radiative effects due to spatial and temporal variations associated with population and surface albedo. The treatment of POA as nonvolatile or semivolatile also influences these efficiencies through different chemical processes. Biogenic OA shows moderate efficiency for health effects and the highest for direct radiative effects but has the lowest efficiency for indirect effects due to the reduced high cloud, caused by stabilized temperature profiles from aerosol-radiation interactions in biogenic OA-rich regions. Biomass burning OA is important for cloud radiative effect changes in remote atmospheres due to its ability to be transported further than other OAs. This study highlights the importance of not only OA characteristics such as toxicity and refractive index but also atmospheric processes such as transport and chemistry in determining health and climate impact efficiencies.

Natural short-lived halogens exert an indirect cooling effect on climate.

Observational evidence shows the ubiquitous presence of ocean-emitted short-lived halogens in the global atmosphere1-3. Natural emissions of these chemical compounds have been anthropogenically amplified since pre-industrial times4-6, while, in addition, anthropogenic short-lived halocarbons are currently being emitted to the atmosphere7,8. Despite their widespread distribution in the atmosphere, the combined impact of these species on Earth's radiative balance remains unknown. Here we show that short-lived halogens exert a substantial indirect cooling effect at present (-0.13 ± 0.03 watts per square metre) that arises from halogen-mediated radiative perturbations of ozone (-0.24 ± 0.02 watts per square metre), compensated by those from methane (+0.09 ± 0.01 watts per square metre), aerosols (+0.03 ± 0.01 watts per square metre) and stratospheric water vapour (+0.011 ± 0.001 watts per square metre). Importantly, this substantial cooling effect has increased since 1750 by -0.05 ± 0.03 watts per square metre (61 per cent), driven by the anthropogenic amplification of natural halogen emissions, and is projected to change further (18-31 per cent by 2100) depending on climate warming projections and socioeconomic development. We conclude that the indirect radiative effect due to short-lived halogens should now be incorporated into climate models to provide a more realistic natural baseline of Earth's climate system.

Evaluating the Impact of Chemical Complexity and Horizontal Resolution on Tropospheric Ozone Over the Conterminous US With a Global Variable Resolution Chemistry Model.

A new configuration of the Community Earth System Model (CESM)/Community Atmosphere Model with full chemistry (CAM-chem) supporting the capability of horizontal mesh refinement through the use of the spectral element (SE) dynamical core is developed and called CESM/CAM-chem-SE. Horizontal mesh refinement in CESM/CAM-chem-SE is unique and novel in that pollutants such as ozone are accurately represented at human exposure relevant scales while also directly including global feedbacks. CESM/CAM-chem-SE with mesh refinement down to ∼14 km over the conterminous US (CONUS) is the beginning of the Multi-Scale Infrastructure for Chemistry and Aerosols (MUSICAv0). Here, MUSICAv0 is evaluated and used to better understand how horizontal resolution and chemical complexity impact ozone and ozone precursors over CONUS as compared to measurements from five aircraft campaigns, which occurred in 2013. This field campaign analysis demonstrates the importance of using finer horizontal resolution to accurately simulate ozone precursors such as nitrogen oxides and carbon monoxide. In general, the impact of using more complex chemistry on ozone and other oxidation products is more pronounced when using finer horizontal resolution where a larger number of chemical regimes are resolved. Large model biases for ozone near the surface remain in the Southeast US as compared to the aircraft observations even with updated chemistry and finer horizontal resolution. This suggests a need for adding the capability of replacing sections of global emission inventories with regional inventories, increasing the vertical resolution in the planetary boundary layer, and reducing model biases in meteorological variables such as temperature and clouds.

Enhanced simulated early 21st century Arctic sea ice loss due to CMIP6 biomass burning emissions.

The mechanisms underlying decadal variability in Arctic sea ice remain actively debated. Here, we show that variability in boreal biomass burning (BB) emissions strongly influences simulated Arctic sea ice on multidecadal time scales. In particular, we find that a strong acceleration in sea ice decline in the early 21st century in the Community Earth System Model version 2 (CESM2) is related to increased variability in prescribed BB emissions in the sixth phase of the Coupled Model Intercomparison Project (CMIP6) through summertime aerosol-cloud interactions. Furthermore, we find that more than half of the reported improvement in sea ice sensitivity to CO2 emissions and global warming from CMIP5 to CMIP6 can be attributed to the increased BB variability, at least in the CESM. These results highlight a new kind of uncertainty that needs to be considered when incorporating new observational data into model forcing while also raising questions about the role of BB emissions on the observed Arctic sea ice loss.

Social science research to inform solar geoengineering.

What are the benefits and drawbacks, and for whom?.

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

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.

Global Changes in Secondary Atmospheric Pollutants During the 2020 COVID-19 Pandemic.

We use the global Community Earth System Model to investigate the response of secondary pollutants (ozone O3, secondary organic aerosols SOA) in different parts of the world in response to modified emissions of primary pollutants during the COVID-19 pandemic. We quantify the respective effects of the reductions in NOx and in volatile organic carbon (VOC) emissions, which, in most cases, affect oxidants in opposite ways. Using model simulations, we show that the level of NOx has been reduced by typically 40% in China during February 2020 and by similar amounts in many areas of Europe and North America in mid-March to mid-April 2020, in good agreement with space and surface observations. We show that, relative to a situation in which the emission reductions are ignored and despite the calculated increase in hydroxyl and peroxy radicals, the ozone concentration increased only in a few NOx-saturated regions (northern China, northern Europe, and the US) during the winter months of the pandemic when the titration of this molecule by NOx was reduced. In other regions, where ozone is NOx-controlled, the concentration of ozone decreased. SOA concentrations decrease in response to the concurrent reduction in the NOx and VOC emissions. The model also shows that atmospheric meteorological anomalies produced substantial variations in the concentrations of chemical species during the pandemic. In Europe, for example, a large fraction of the ozone increase in February 2020 was associated with meteorological anomalies, while in the North China Plain, enhanced ozone concentrations resulted primarily from reduced emissions of primary pollutants.

Toward practical stratospheric aerosol albedo modification: Solar-powered lofting.

Many climate intervention (CI) methods have been proposed to offset greenhouse gas-induced global warming, but the practicalities regarding implementation have not received sufficient attention. Stratospheric aerosol injection (SAI) involves introducing large amounts of CI material well within the stratosphere to enhance the aerosol loading, thereby increasing reflection of solar radiation. We explore a delivery method termed solar-powered lofting (SPL) that uses solar energy to loft CI material injected at lower altitudes accessible by conventional aircraft. Particles that absorb solar radiation are dispersed with the CI material and heat the surrounding air. The heated air rises, carrying the CI material to the stratosphere. Global model simulations show that black carbon aerosol (10 microgram per cubic meter) is sufficient to quickly loft CI material well into the stratosphere. SPL could make SAI viable at present, is also more energy efficient, and disperses CI material faster than direct stratospheric injection.

Potential ecological impacts of climate intervention by reflecting sunlight to cool Earth.

As the effects of anthropogenic climate change become more severe, several approaches for deliberate climate intervention to reduce or stabilize Earth's surface temperature have been proposed. Solar radiation modification (SRM) is one potential approach to partially counteract anthropogenic warming by reflecting a small proportion of the incoming solar radiation to increase Earth's albedo. While climate science research has focused on the predicted climate effects of SRM, almost no studies have investigated the impacts that SRM would have on ecological systems. The impacts and risks posed by SRM would vary by implementation scenario, anthropogenic climate effects, geographic region, and by ecosystem, community, population, and organism. Complex interactions among Earth's climate system and living systems would further affect SRM impacts and risks. We focus here on stratospheric aerosol intervention (SAI), a well-studied and relatively feasible SRM scheme that is likely to have a large impact on Earth's surface temperature. We outline current gaps in knowledge about both helpful and harmful predicted effects of SAI on ecological systems. Desired ecological outcomes might also inform development of future SAI implementation scenarios. In addition to filling these knowledge gaps, increased collaboration between ecologists and climate scientists would identify a common set of SAI research goals and improve the communication about potential SAI impacts and risks with the public. Without this collaboration, forecasts of SAI impacts will overlook potential effects on biodiversity and ecosystem services for humanity.

Intercomparison Between Surrogate, Explicit, and Full Treatments of VSL Bromine Chemistry Within the CAM-Chem Chemistry-Climate Model.

Many Chemistry-Climate Models (CCMs) include a simplified treatment of brominated very short-lived (VSLBr) species by assuming CH3Br as a surrogate for VSLBr. However, neglecting a comprehensive treatment of VSLBr in CCMs may yield an unrealistic representation of the associated impacts. Here, we use the Community Atmospheric Model with Chemistry (CAM-Chem) CCM to quantify the tropospheric and stratospheric changes between various VSLBr chemical approaches with increasing degrees of complexity (i.e., surrogate, explicit, and full). Our CAM-Chem results highlight the improved accuracy achieved by considering a detailed treatment of VSLBr photochemistry, including sea-salt aerosol dehalogenation and heterogeneous recycling on ice-crystals. Differences between the full and surrogate schemes maximize in the lowermost stratosphere and midlatitude free troposphere, resulting in a latitudinally dependent reduction of ∼1-7 DU in total ozone column and a ∼5%-15% decrease of the OH/HO2 ratio. We encourage all CCMs to include a complete chemical treatment of VSLBr in the troposphere and stratosphere.

Mapping Yearly Fine Resolution Global Surface Ozone through the Bayesian Maximum Entropy Data Fusion of Observations and Model Output for 1990-2017.

Estimates of ground-level ozone concentrations are necessary to determine the human health burden of ozone. To support the Global Burden of Disease Study, we produce yearly fine resolution global surface ozone estimates from 1990 to 2017 through a data fusion of observations and models. As ozone observations are sparse in many populated regions, we use a novel combination of the M3Fusion and Bayesian Maximum Entropy (BME) methods. With M3Fusion, we create a multimodel composite by bias-correcting and weighting nine global atmospheric chemistry models based on their ability to predict observations (8834 sites globally) in each region and year. BME is then used to integrate observations, such that estimates match observations at each monitoring site with the observational influence decreasing smoothly across space and time until the output matches the multimodel composite. After estimating at 0.5° resolution using BME, we add fine spatial detail from an additional model, yielding estimates at 0.1° resolution. Observed ozone is predicted more accurately (R2 = 0.81 at the test point, 0.63 at 0.1°, and 0.62 at 0.5°) than the multimodel mean (R2 = 0.28 at 0.5°). Global ozone exposure is estimated to be increasing, driven by highly populated regions of Asia and Africa, despite decreases in the United States and Russia.

The role of tropical volcanic eruptions in exacerbating Indian droughts.

The Indian summer monsoon rainfall (ISMR) is vital for the livelihood of millions of people in the Indian region; droughts caused by monsoon failures often resulted in famines. Large volcanic eruptions have been linked with reductions in ISMR, but the responsible mechanisms remain unclear. Here, using 145-year (1871-2016) records of volcanic eruptions and ISMR, we show that ISMR deficits prevail for two years after moderate and large (VEI > 3) tropical volcanic eruptions; this is not the case for extra-tropical eruptions. Moreover, tropical volcanic eruptions strengthen El Niño and weaken La Niña conditions, further enhancing Indian droughts. Using climate-model simulations of the 2011 Nabro volcanic eruption, we show that eruption induced an El Niño like warming in the central Pacific for two consecutive years due to Kelvin wave dissipation triggered by the eruption. This El Niño like warming in the central Pacific led to a precipitation reduction in the Indian region. In addition, solar dimming caused by the volcanic plume in 2011 reduced Indian rainfall.

Global airborne sampling reveals a previously unobserved dimethyl sulfide oxidation mechanism in the marine atmosphere.

Dimethyl sulfide (DMS), emitted from the oceans, is the most abundant biological source of sulfur to the marine atmosphere. Atmospheric DMS is oxidized to condensable products that form secondary aerosols that affect Earth's radiative balance by scattering solar radiation and serving as cloud condensation nuclei. We report the atmospheric discovery of a previously unquantified DMS oxidation product, hydroperoxymethyl thioformate (HPMTF, HOOCH2SCHO), identified through global-scale airborne observations that demonstrate it to be a major reservoir of marine sulfur. Observationally constrained model results show that more than 30% of oceanic DMS emitted to the atmosphere forms HPMTF. Coincident particle measurements suggest a strong link between HPMTF concentration and new particle formation and growth. Analyses of these observations show that HPMTF chemistry must be included in atmospheric models to improve representation of key linkages between the biogeochemistry of the ocean, marine aerosol formation and growth, and their combined effects on climate.

Correcting model biases of CO in East Asia: impact on oxidant distributions during KORUS-AQ.

Global coupled chemistry-climate models underestimate carbon monoxide (CO) in the Northern Hemisphere, exhibiting a pervasive negative bias against measurements peaking in late winter and early spring. While this bias has been commonly attributed to underestimation of direct anthropogenic and biomass burning emissions, chemical production and loss via OH reaction from emissions of anthropogenic and biogenic volatile organic compounds (VOCs) play an important role. Here we investigate the reasons for this underestimation using aircraft measurements taken in May and June 2016 from the Korea-United States Air Quality (KORUS-AQ) experiment in South Korea and the Air Chemistry Research in Asia (ARIAs) in the North China Plain (NCP). For reference, multispectral CO retrievals (V8J) from the Measurements of Pollution in the Troposphere (MOPITT) are jointly assimilated with meteorological observations using an ensemble adjustment Kalman filter (EAKF) within the global Community Atmosphere Model with Chemistry (CAM-Chem) and the Data Assimilation Research Testbed (DART). With regard to KORUS-AQ data, CO is underestimated by 42% in the control run and by 12% with the MOPITT assimilation run. The inversion suggests an underestimation of anthropogenic CO sources in many regions, by up to 80% for northern China, with large increments over the Liaoning Province and the North China Plain (NCP). Yet, an often-overlooked aspect of these inversions is that correcting the underestimation in anthropogenic CO emissions also improves the comparison with observational O3 datasets and observationally constrained box model simulations of OH and HO2. Running a CAM-Chem simulation with the updated emissions of anthropogenic CO reduces the bias by 29% for CO, 18% for ozone, 11% for HO2, and 27% for OH. Longer-lived anthropogenic VOCs whose model errors are correlated with CO are also improved, while short-lived VOCs, including formaldehyde, are difficult to constrain solely by assimilating satellite retrievals of CO. During an anticyclonic episode, better simulation of O3, with an average underestimation of 5.5 ppbv, and a reduction in the bias of surface formaldehyde and oxygenated VOCs can be achieved by separately increasing by a factor of 2 the modeled biogenic emissions for the plant functional types found in Korea. Results also suggest that controlling VOC and CO emissions, in addition to widespread NO x controls, can improve ozone pollution over East Asia.

Atmospheric Acetaldehyde: Importance of Air-Sea Exchange and a Missing Source in the Remote Troposphere.

We report airborne measurements of acetaldehyde (CH3CHO) during the first and second deployments of the National Aeronautics and Space Administration (NASA) Atmospheric Tomography Mission (ATom). The budget of CH3CHO is examined using the Community Atmospheric Model with chemistry (CAM-chem), with a newly-developed online air-sea exchange module. The upper limit of the global ocean net emission of CH3CHO is estimated to be 34 Tg a-1 (42 Tg a-1 if considering bubble-mediated transfer), and the ocean impacts on tropospheric CH3CHO are mostly confined to the marine boundary layer. Our analysis suggests that there is an unaccounted CH3CHO source in the remote troposphere and that organic aerosols can only provide a fraction of this missing source. We propose that peroxyacetic acid (PAA) is an ideal indicator of the rapid CH3CHO production in the remote troposphere. The higher-than-expected CH3CHO measurements represent a missing sink of hydroxyl radicals (and halogen radical) in current chemistry-climate models.

Tropospheric ozone in CCMI models and Gaussian process emulation to understand biases in the SOCOLv3 chemistry-climate model.

Previous multi-model intercomparisons have shown that chemistry-climate models exhibit significant biases in tropospheric ozone compared with observations. We investigate annual-mean tropospheric column ozone in 15 models participating in the SPARC/IGAC (Stratosphere-troposphere Processes and their Role in Climate/International Global Atmospheric Chemistry) Chemistry-Climate Model Initiative (CCMI). These models exhibit a positive bias, on average, of up to 40-50% in the Northern Hemisphere compared with observations derived from the Ozone Monitoring Instrument and Microwave Limb Sounder (OMI/MLS), and a negative bias of up to ~30% in the Southern Hemisphere. SOCOLv3.0 (version 3 of the Solar-Climate Ozone Links CCM), which participated in CCMI, simulates global-mean tropospheric ozone columns of 40.2 DU - approximately 33% larger than the CCMI multi-model mean. Here we introduce an updated version of SOCOLv3.0, "SOCOLv3.1", which includes an improved treatment of ozone sink processes, and results in a reduction in the tropospheric column ozone bias of up to 8 DU, mostly due to the inclusion of N2O5 hydrolysis on tropospheric aerosols. As a result of these developments, tropospheric column ozone amounts simulated by SOCOLv3.1 are comparable with several other CCMI models. We apply Gaussian process emulation and sensitivity analysis to understand the remaining ozone bias in SOCOLv3.1. This shows that ozone precursors (nitrogen oxides (NOx), carbon monoxide, methane and other volatile organic compounds) are responsible for more than 90% of the variance in tropospheric ozone. However, it may not be the emissions inventories themselves that result in the bias, but how the emissions are handled in SOCOLv3.1, and we discuss this in the wider context of the other CCMI models. Given that the emissions data set to be used for phase 6 of the Coupled Model Intercomparison Project includes approximately 20% more NOx than the data set used for CCMI, further work is urgently needed to address the challenges of simulating sub-grid processes of importance to tropospheric ozone in the current generation of chemistry-climate models.

The Simulation of Stratospheric Water Vapor over the Asian Summer Monsoon Region in CESM1(WACCM) Models.

Previous observational studies have found a persistent maximum in stratospheric water vapor (SWV) in the upper troposphere lower stratosphere (UTLS) confined by the upper-level anticyclone over the Asian summer monsoon region. This study investigates the simulation of SWV in the Whole Atmosphere Community Climate Model (WACCM). WACCM generally tends to simulate a SWV maximum over the central Pacific Ocean, but this bias is largely improved in the high vertical resolution version. The high vertical resolution model with increased vertical layers in the UTLS is found to have a less stratified UTLS over the central Pacific Ocean compared with the low vertical resolution model. It therefore simulates a steepened PV gradient over the central Pacific Ocean that better closes the upper-level anticyclone and confines the SWV within the enhanced transport barrier.