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The NASA ACTIVATE Mission

The NASA Aerosol Cloud Meteorology Interactions over the Western Atlantic Experiment (ACTIVATE) conducted 162 joint flights with two aircraft over the northwest Atlantic to study aerosol–cloud interactions (ACIs), which represent the largest uncertainty in estimating total anthropogenic radiative forcing. The combination of a high-flying King Air and low-flying HU-25 Falcon, equipped with remote sensing and in situ instruments, characterized trace gases, aerosol particles, clouds, and meteorological variables with data collected nearly simultaneously below, within, and above marine boundary layer (MBL) clouds. Flights spanning warm and cold seasons across 3 years (2020–22) provided a broad range of conditions associated with aerosol particles, cloud properties (including particle size and phase), and meteorology, ideally suited for robust ACI calculations and assessing how well models simulate a wide range of MBL clouds from stratiform to cumulus. ACTIVATE data suggest that drivers of cloud droplet number concentration N d , including aerosol particles and MBL dynamics, vary between winter and summer months with a stronger potential to convert aerosol particles into cloud droplets in winter. Models of varying complexity not only highlight some skills in simulating winter and summer cloud types but also identify challenges that still need to be addressed such as treatment of turbulence, wet scavenging, and mesoscale organization. Remote sensing advances range from new retrieval methods for N d , cloud phase classification, vertically resolved aerosol and cloud condensation nuclei number concentration, and ocean surface wind speed. This work describes these scientific and technological advances along with efforts in outreach and open data science.

aerosol indirect effect↗

Distinct responses of Asian summer monsoon to black carbon aerosols and greenhouse gases

Black carbon (BC) aerosols emitted from natural and anthropogenic sources induce positive radiative forcing and global warming, which in turn significantly affect the Asian summer monsoon (ASM). However, many aspects of the BC effect on the ASM remain elusive and largely inconsistent among previous studies, which is strongly dependent on different low-level thermal feedbacks over the Asian continent and the surrounding ocean. This study examines the response of the ASM to BC forcing in comparison with the effect of doubled greenhouse gases (GHGs) by analyzing the Precipitation Driver Response Model Intercomparison Project (PDRMIP) simulations under an extremely high BC level (10 times modern global BC emissions or concentrations, labeled BC×10) from nine global climate models (GCMs). The results show that although BC and GHGs both enhance the ASM precipitation minus evaporation (P–E; a 13.6 % increase for BC forcing and 12.1 % for GHGs from the nine-model ensemble, respectively), there exists a much larger uncertainty in changes in ASM P–E induced by BC than by GHGs. The summer P–E is increased by 7.7 % to 15.3 % due to these two forcings over three subregions, including East Asian, South Asian and western North Pacific monsoon regions. Further analysis of moisture budget reveals distinct mechanisms controlling the increases in ASM P–E induced by BC and GHGs. The change in ASM P–E by BC is dominated by the dynamic effect due to the enhanced large-scale monsoon circulation, whereas the GHG-induced change is dominated by the thermodynamic effect through increasing atmospheric water vapor. Radiative forcing of BC significantly increases the upper-level atmospheric temperature over the Asian region to enhance the upper-level meridional land–sea thermal gradient (MLOTG), resulting in a northward shift of the upper-level subtropical westerly jet and an enhancement of the low-level monsoon circulation, whereas radiative forcing of GHGs significantly increases the tropical upper-level temperature, which reduces the upper-level MLOTG and suppresses the low-level monsoonal circulation. Hence, our results indicate a different mechanism of BC climate effects under the extremely high BC level: that BC forcing significantly enhances the upper-level atmospheric temperature over the Asian region, determining ASM changes, instead of low-level thermal feedbacks as indicated by previous studies.

54 ENVIRONMENTAL SCIENCES↗

Distinct responses of Asian summer monsoon to black carbon aerosols and greenhouse gases

Black carbon (BC) aerosols emitted from natural and anthropogenic sources induce positive radiative forcing and global warming, which in turn significantly affect the Asian summer monsoon (ASM). However, many aspects of the BC effect on ASM remain elusive and largely inconsistent among previous studies, which is strongly dependent on different low-level thermal feedbacks over the Asian continent and the surrounding ocean. This study examines the response of ASM to BC forcing in comparison with the effect of doubled greenhouse gases (GHGs) by analyzing the Precipitation Driver Response Model Intercomparison Project (PDRMIP) simulations under an extreme high BC level (10 times modern global BC emissions or concentrations, labeled by BC $\times$ 10) from nine global climate models (GCMs). The results show that although BC and GHGs both enhance the ASM precipitation minus evaporation (P–E) (a 13.6 % increase for BC forcing and 12.1 % for GHGs from the nine-model ensemble, respectively), there exists a much larger uncertainty in changes in ASM P–E induced by BC than by GHGs. The summer P–E is increased by 7.7 % to 15.3 % due to these two forcings over three sub-regions including East Asian, South Asian, and western North Pacific monsoon regions. Further analysis of moisture budget reveals distinct mechanisms controlling the increases in ASM P–E induced by BC and GHGs. The change in ASM P–E by BC is dominated by the dynamic effect due to the enhanced large-scale monsoon circulation, whereas the GHG-induced change is dominated by the thermodynamic effect through increasing atmospheric water vapor. Radiative forcing of BC significantly increases the upper-level atmospheric temperature over the Asian region to enhance the upper-level meridional land-sea thermal gradient (MLOTG), resulting in a northward shift of the upper-level subtropical westerly jet and an enhancement of the low-level monsoon circulation; whereas radiative forcing of GHGs significantly increases the tropical upper-level temperature, which reduces the upper-level MLOTG and suppresses the low-level monsoonal circulation. Hence, our results indicate a different mechanism of BC climate effects under the extreme high BC level, that BC forcing significantly enhances the upper-level atmospheric temperature over the Asian region, determining ASM changes, instead of low-level thermal feedbacks as indicated by previous studies.

54 ENVIRONMENTAL SCIENCES↗

Understanding aerosol–cloud interactions using a single-column model for a cold-air outbreak case during the ACTIVATE campaign

Marine boundary layer clouds play a critical role in Earth's energy balance. Their microphysical and radiative properties are highly impacted by ambient aerosols and dynamic forcings. In this study, we evaluate the representation of these clouds and related aerosol–cloud interaction processes in the single-column version of the E3SM climate model (SCM) against field measurements collected during the NASA ACTIVATE campaign over the western North Atlantic, as well as intercompare results with high-resolution process level models. We show that E3SM SCM reproduces the macrophysical properties of post-frontal boundary layer clouds in a cold-air outbreak (CAO) case well. However, it generates fewer but larger cloud droplets compared to aircraft measurements. Further sensitivity tests show that the underestimation of both aerosol number concentration and vertical velocity variance contributes to this bias. Aerosol–cloud interactions are examined by perturbing prescribed aerosol properties in E3SM SCM with fixed dynamics. Higher aerosol number concentration or hygroscopicity leads to more numerous but smaller cloud droplets, resulting in a stronger cooling via shortwave cloud forcing. This apparent Twomey effect is consistent with prior climate model studies. The cloud liquid water path shows a weakly positive relation with cloud droplet number concentration due to precipitation suppression. This weak aerosol effect on cloud macrophysics may be attributed to the dominant impact of strong dynamical forcing associated with the CAO. Our findings indicate that the SCM framework is a key tool to bridge the gap between climate models, process level models, and field observations to facilitate process level understanding.

54 ENVIRONMENTAL SCIENCES↗

Harnessing stratospheric diffusion barriers for enhanced climate geoengineering

Stratospheric sulfate aerosol geoengineering is a proposed method to temporarily intervene in the climate system to increase the reflectance of shortwave radiation and reduce mean global temperature. In previous climate modeling studies, choosing injection locations for geoengineering aerosols has, thus far, only utilized the average dynamics of stratospheric wind fields instead of accounting for the essential role of time-varying material transport barriers in turbulent atmospheric flows. Here we conduct the first analysis of sulfate aerosol dispersion in the stratosphere, comparing what is now a standard fixed-injection scheme with time-varying injection locations that harness short-term stratospheric diffusion barriers. We show how diffusive transport barriers can quickly be identified, and we provide an automated injection location selection algorithm using short forecast and reanalysis data. Within the first 7 d days of transport, the dynamics-based approach is able to produce particle distributions with greater global coverage than fixed-site methods with fewer injections. Additionally, this enhanced dispersion slows aerosol microphysical growth and can reduce the effective radii of aerosols up to 200–300 d after injection. While the long-term dynamics of aerosol dispersion are accurately predicted with transport barriers calculated from short forecasts, the long-term influence on radiative forcing is more difficult to predict and warrants deeper investigation. Statistically significant changes in radiative forcing at timescales beyond the forecasting window showed mixed results, potentially increasing or decreasing forcing after 1 year when compared to fixed injections. We conclude that future feasibility studies of geoengineering should consider the cooling benefits possible by strategically injecting sulfate aerosols at optimized time-varying locations. Our method of utilizing time-varying attracting and repelling structures shows great promise for identifying optimal dispersion locations, and radiative forcing impacts can be improved by considering additional meteorological variables.

54 ENVIRONMENTAL SCIENCES↗

Observationally constrained analysis of sulfur cycle in the marine atmosphere with NASA ATom measurements and AeroCom model simulations

The atmospheric sulfur cycle plays a key role in air quality, climate, and ecosystems, such as pollution, radiative forcing, new particle formation, and acid rain. In this study, we compare the spatially and temporally resolved measurements from the NASA Atmospheric Tomography (ATom) mission with simulations from five AeroCom III models for four sulfur species (dimethyl sulfide (DMS), sulfur dioxide (SO 2 ), particulate methanesulfonate (MSA), and particulate sulfate (SO 4 )). We focus on remote regions over the Pacific, Atlantic, and Southern oceans from near the surface to ~12 km altitude range covering all four seasons. In general, the differences among model results can be greater than 1 order of magnitude. Comparing with observations, model-simulated SO 2 is generally low, whereas SO 4 is generally high. Simulated DMS concentrations near the sea surface exceed observed levels by a factor of 5 in most cases, suggesting potential overestimation of DMS emissions in all models. With GEOS model simulations of tagging emission from anthropogenic, biomass burning, volcanic, and oceanic sources, we find that anthropogenic emissions are the dominant source of sulfate aerosol (40 %–60 % of the total amount) in the ATom measurements at almost all altitudes, followed by volcanic emissions (18 %–32 %) and oceanic sources (16 %–32 %). Similar source contributions can also be derived at broad ocean basins and on monthly scales, indicating the representativeness of ATom measurements for global ocean. Our work presents the first assessment of AeroCom sulfur study using ATom measurements, providing directions for improving sulfate simulations, which remain the largest uncertainty in radiative forcing estimates in aerosol climate models.

54 ENVIRONMENTAL SCIENCES↗

Bridging New Observational Capabilities and Process-Level Simulation: Insights into Aerosol Roles in the Earth System

The spatial distribution of ambient aerosol particles significantly impacts aerosol–radiation–cloud interactions, which contribute to the largest uncertainty in global anthropogenic radiative forcing estimations. However, the atmospheric boundary layer and lower free troposphere have not been adequately sampled in terms of spatiotemporal resolution, hindering a comprehensive characterization of various atmospheric processes and impeding our understanding of the Earth system. To address this research data gap, we have leveraged the development of uncrewed aerial systems (UAS) and advanced measurement techniques to obtain mesoscale spatial data on aerosol microphysical and optical properties around the U.S. Southern Great Plains (SGP) atmospheric observatory. Our study also benefits from state-of-the-art laboratory facilities that include three-dimensional molecular imaging techniques enabled by secondary ion mass spectrometry and nanogram-level chemical composition analysis via micronebulization aerosol mass spectrometry. Through our study, we have developed a framework for observation–modeling integration, enabling an examination of how various assumptions about the organic–inorganic components mixing state, inferred from chemical analysis, affect clouds and radiation in observation-constrained model simulations. By integrating observational constraints (derived from offline chemical analysis of the aerosol surface using collected samples) with in situ UAS observations, we have identified a prominent role of organic-enriched nanometer layers located at the surface of aerosol particles in determining profiles of aerosol optical and hygroscopic properties over the SGP observatory. Furthermore, we have improved the agreement between predicted clouds and ground-based cloud lidar measurements. This UAS–model–laboratory integration exemplifies how these new advanced capabilities can significantly enhance our understanding of aerosol–radiation–cloud interactions.

54 ENVIRONMENTAL SCIENCES↗

Buffering of Aerosol-Cloud Adjustments by Coupling Between Radiative Susceptibility and Precipitation Efficiency

Aerosol-cloud interactions (ACI) in warm clouds are the primary source of uncertainty in effective radiative forcing (ERF) during the historical period and, by extension, inferred climate sensitivity. The ERF due to ACI (ERFaci) is composed of the radiative forcing due to changes in cloud microphysics and cloud adjustments to microphysics. Here, we examine the processes that drive ERFaci using a perturbed parameter ensemble (PPE) hosted in CAM6. Observational constraints on the PPE result in substantial constraints in the response of cloud microphysics and macrophysics to anthropogenic aerosol, but only minimal constraint on ERFaci. Examination of cloud and radiation processes in the PPE reveal buffering of ERFaci by the interaction of precipitation efficiency and radiative susceptibility.

54 ENVIRONMENTAL SCIENCES↗

CMIP7 Data Request: atmosphere priorities and opportunities

This paper presents a comprehensive overview of the Coupled Model Intercomparison Project Phase 7 (CMIP7) request for data unlocking key research avenues in atmospheric science and provides justification for the resources needed to produce this data. Topics within the CMIP7 Atmosphere Theme centre around processes and feedbacks in atmospheric science such as clouds, aerosols and atmospheric chemistry, atmospheric circulation, temperature variability and extremes, radiative forcings, and Earth system model evaluation. These topics are summarised in this paper as scientific “opportunities” which will be realised through CMIP7 experiments and Earth system model outputs. These opportunities were submitted by a thematic group of atmospheric science community representatives combined with an extended consultation process. The production of these variables will close key gaps and uncertainties identified during previous rounds of CMIP, and will be broadly used by scientific, policy, governmental, industry, and other communities that rely on climate model projections for research and decision making, including supporting the 7th Intergovernmental Panel on Climate Change Assessment Report (AR7). As an author group, we also reflect on the process used to collate this data request and make recommendations to future CMIP governance on implementing a consultation on this scale in the future.

58 GEOSCIENCES↗

Revisiting particle dry deposition and its role in radiative effect estimates

Wet and dry deposition remove aerosols from the atmosphere, and these processes control aerosol lifetime and thus impact climate and air quality. Dry deposition is a significant source of aerosol uncertainty in global chemical transport and climate models. Dry deposition parameterizations in most global models were developed when few particle deposition measurements were available. However, new measurement techniques have enabled more size-resolved particle flux observations. We combined literature measurements with data that we collected over a grassland in Oklahoma and a pine forest in Colorado to develop a dry deposition parameterization. We find that relative to observations, previous parameterizations overestimated deposition of the accumulation and Aitken mode particles, and underestimated in the coarse mode. These systematic differences in observed and modeled accumulation mode particle deposition velocities are as large as an order of magnitude over terrestrial ecosystems. As accumulation mode particles form most of the cloud condensation nuclei (CCN) that influence the indirect radiative effect, this model-measurement discrepancy in dry deposition alters modeled CCN and radiative forcing. We present a revised observationally driven parameterization for regional and global aerosol models. Using this revised dry deposition scheme in the Goddard Earth Observing System (GEOS)-Chem chemical transport model, we find that global surface accumulation-mode number concentrations increase by 62% and enhance the global combined anthropogenic and natural aerosol indirect effect by −0.63 W m −2 . Our observationally constrained approach should reduce the uncertainty of particle dry deposition in global chemical transport models.

54 ENVIRONMENTAL SCIENCES↗

Modeled and observed properties related to the direct aerosol radiative effect of biomass burning aerosol over the southeastern Atlantic

Biomass burning smoke is advected over the southeastern Atlantic Ocean between July and October of each year. This smoke plume overlies and mixes into a region of persistent low marine clouds. Model calculations of climate forcing by this plume vary significantly in both magnitude and sign. NASA EVS-2 (Earth Venture Suborbital-2) ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) had deployments for field campaigns off the west coast of Africa in 3 consecutive years (September 2016, August 2017, and October 2018) with the goal of better characterizing this plume as a function of the monthly evolution by measuring the parameters necessary to calculate the direct aerosol radiative effect. Here, this dataset and satellite retrievals of cloud properties are used to test the representation of the smoke plume and the underlying cloud layer in two regional models (WRF-CAM5 and CNRM-ALADIN) and two global models (GEOS and UM-UKCA). The focus is on the comparisons of those aerosol and cloud properties that are the primary determinants of the direct aerosol radiative effect and on the vertical distribution of the plume and its properties. The representativeness of the observations to monthly averages are tested for each field campaign, with the sampled mean aerosol light extinction generally found to be within 20 % of the monthly mean at plume altitudes. When compared to the observations, in all models, the simulated plume is too vertically diffuse and has smaller vertical gradients, and in two of the models (GEOS and UM-UKCA), the plume core is displaced lower than in the observations. Plume carbon monoxide, black carbon, and organic aerosol masses indicate underestimates in modeled plume concentrations, leading, in general, to underestimates in mid-visible aerosol extinction and optical depth. Biases in mid-visible single scatter albedo are both positive and negative across the models. Observed vertical gradients in single scatter albedo are not captured by the models, but the models do capture the coarse temporal evolution, correctly simulating higher values in October (2018) than in August (2017) and September (2016). Uncertainties in the measured absorption Ångstrom exponent were large but propagate into a negligible (<4 %) uncertainty in integrated solar absorption by the aerosol and, therefore, in the aerosol direct radiative effect. Model biases in cloud fraction, and, therefore, the scene albedo below the plume, vary significantly across the four models. The optical thickness of clouds is, on average, well simulated in the WRF-CAM5 and ALADIN models in the stratocumulus region and is underestimated in the GEOS model; UM-UKCA simulates cloud optical thickness that is significantly too high. Overall, the study demonstrates the utility of repeated, semi-random sampling across multiple years that can give insights into model biases and how these biases affect modeled climate forcing. The combined impact of these aerosol and cloud biases on the direct aerosol radiative effect (DARE) is estimated using a first-order approximation for a subset of five comparison grid boxes. A significant finding is that the observed grid box average aerosol and cloud properties yield a positive (warming) aerosol direct radiative effect for all five grid boxes, whereas DARE using the grid-box-averaged modeled properties ranges from much larger positive values to small, negative values. It is shown quantitatively how model biases can offset each other, so that model improvements that reduce biases in only one property (e.g., single scatter albedo but not cloud fraction) would lead to even greater biases in DARE. Across the models, biases in aerosol extinction and in cloud fraction and optical depth contribute the largest biases in DARE, with aerosol single scatter albedo also making a significant contribution.

54 ENVIRONMENTAL SCIENCES↗

Cloud condensation nuclei concentrations derived from the CAMS reanalysis

Determining number concentrations of cloud condensation nuclei (CCN) is one of the first steps in the chain in analysis of cloud droplet formation, the direct microphysical link between aerosols and cloud droplets, and a process key for aerosol–cloud interactions (ACI). However, due to sparse coverage of in situ measurements and difficulties associated with retrievals from satellites, a global exploration of their magnitude, source as well as temporal and spatial distribution cannot be easily obtained. Thus, a better representation of CCN numbers is one of the goals for quantifying ACI processes and achieving uncertainty-reduced estimates of their associated radiative forcing. Here, we introduce a new CCN dataset which is derived based on aerosol mass mixing ratios from the latest Copernicus Atmosphere Monitoring Service reanalysis (CAMSRA) in a diagnostic model that uses CAMSRA aerosol properties and a simplified kappa-Köhler framework suitable for global models. The emitted aerosols in CAMSRA are not only based on input from emission inventories using aerosol observations, they also have a strong tie to satellite-retrieved aerosol optical depth (AOD) as this is assimilated as a constraining factor in the reanalysis. Furthermore, the reanalysis interpolates for cases of poor or missing retrievals and thus allows for a full spatiotemporal quantification of CCN numbers. The derived CCN dataset captures the general trend and spatial and temporal distribution of total CCN number concentrations and CCN from different aerosol species. A brief evaluation with ground-based in situ measurements demonstrates the improvement of the modelled CCN over the sole use of AOD as a proxy for CCN as the overall correlation coefficient improved from 0.37 to 0.71. However, we find the modelled CCN from CAMSRA to be generally high biased and find a particular erroneous overestimation at one heavily polluted site which emphasises the need for further validation. The CCN dataset (https://doi.org/10.26050/WDCC/QUAERERE_CCNCAMS_v1, Block, 2023), which is now freely available to users, features 3-D CCN number concentrations of global coverage for various supersaturations and aerosol species covering the years 2003–2021 with daily frequency. This dataset is one of its kind as it offers lots of opportunities to be used for evaluation in models and in ACI studies.

54 ENVIRONMENTAL SCIENCES↗

Abrupt reduction in shipping emission as an inadvertent geoengineering termination shock produces substantial radiative warming

Abstract Human activities affect the Earth’s climate through modifying the composition of the atmosphere, which then creates radiative forcing that drives climate change. The warming effect of anthropogenic greenhouse gases has been partially balanced by the cooling effect of anthropogenic aerosols. In 2020, fuel regulations abruptly reduced the emission of sulfur dioxide from international shipping by about 80% and created an inadvertent geoengineering termination shock with global impact. Here we estimate the regulation leads to a radiative forcing of $$+0.2\pm 0.11$$ + 0.2 ± 0.11 Wm −2 averaged over the global ocean. The amount of radiative forcing could lead to a doubling (or more) of the warming rate in the 2020 s compared with the rate since 1980 with strong spatiotemporal heterogeneity. The warming effect is consistent with the recent observed strong warming in 2023 and expected to make the 2020 s anomalously warm. The forcing is equivalent in magnitude to 80% of the measured increase in planetary heat uptake since 2020. The radiative forcing also has strong hemispheric contrast, which has important implications for precipitation pattern changes. Our result suggests marine cloud brightening may be a viable geoengineering method in temporarily cooling the climate that has its unique challenges due to inherent spatiotemporal heterogeneity.

54 ENVIRONMENTAL SCIENCES↗

Effects of marine organic aerosols as sources of immersion-mode ice-nucleating particles on high-latitude mixed-phase clouds

Mixed-phase clouds are frequently observed in high-latitude regions and have important impacts on the surface energy budget and regional climate. Marine organic aerosol (MOA), a natural source of aerosol emitted over ~70 % of Earth's surface, may significantly modify the properties and radiative forcing of mixed-phase clouds. However, the relative importance of MOA as a source of ice-nucleating particles (INPs) in comparison to mineral dust, and MOA's effects as cloud condensation nuclei (CCN) and INPs on mixed-phase clouds are still open questions. In this study, we implement MOA as a new aerosol species into the Community Atmosphere Model version 6 (CAM6), the atmosphere component of the Community Earth System Model version 2 (CESM2), and allow the treatment of aerosol–cloud interactions of MOA via droplet activation and ice nucleation. CAM6 reproduces observed seasonal cycles of marine organic matter at Mace Head and Amsterdam Island when the MOA fraction of sea spray aerosol in the model is assumed to depend on sea spray biology but fails when this fraction is assumed to be constant. Model results indicate that marine INPs dominate primary ice nucleation below 400 hPa over the Southern Ocean and Arctic boundary layer, while dust INPs are more abundant elsewhere. By acting as CCN, MOA exerts a shortwave cloud forcing change of -2.78 W m-2 over the Southern Ocean in the austral summer. By acting as INPs, MOA enhances the longwave cloud forcing by 0.35 W m-2 over the Southern Ocean in the austral winter. The annual global mean net cloud forcing changes due to CCN and INPs of MOA are -0.35 and 0.016 W m-2, respectively. These findings highlight the vital importance for Earth system models to consider MOA as an important aerosol species for the interactions of biogeochemistry, hydrological cycle, and climate change.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Constraining effects of aerosol-cloud interaction by accounting for coupling between cloud and land surface

Aerosol-cloud interactions (ACIs) are vital for regulating Earth’s climate by influencing energy and water cycles. Yet, effects of ACI bear large uncertainties, evidenced by systematic discrepancies between observed and modeled estimates. This study quantifies a major bias in ACI determinations, stemming from conventional surface or space measurements that fail to capture aerosol at the cloud level unless the cloud is coupled with land surface. We introduce an advanced approach to determine radiative forcing of ACI by accounting for cloud-surface coupling. By integrating field observations, satellite data, and model simulations, this approach reveals a drastic alteration in aerosol vertical transport and ACI effects caused by cloud coupling. In coupled regimes, aerosols enhance cloud droplet number concentration across the boundary layer more homogeneously than in decoupled conditions, under which aerosols from the free atmosphere predominantly affect cloud properties, leading to marked cooling effects. Our findings spotlight cloud-surface coupling as a key factor for ACI quantification, hinting at potential underassessments in traditional estimates.

54 ENVIRONMENTAL SCIENCES↗

Global Dust Cycle and Direct Radiative Effect in E3SM Version 1: Impact of Increasing Model Resolution

Quantification of dust aerosols in Earth System Models (ESMs) has important implications for water cycle and biogeochemistry studies. This study examines the global life cycle and direct radiative effects (DREs) of dust in the U.S. Department of Energy's Energy Exascale Earth System Model version 1 (E3SMv1), and the impact of increasing model resolution both horizontally and vertically. The default 1° E3SMv1 captures the spatial and temporal variability in the observed dust aerosol optical depth (DAOD) reasonably well, but overpredicts dust absorption in the shortwave (SW). Simulations underestimate the dust vertical and long-range transport, compared with the satellite dust extinction profiles. After updating dust refractive indices and correcting for a bias in partitioning size-segregated emissions, both SW cooling and longwave (LW) warming of dust simulated by E3SMv1 are increased and agree better with other recent studies. The estimated net dust DRE of –0.42 Wm –2 represents a stronger cooling effect than the observationally based estimate –0.2 Wm –2 (–0.48 to +0.2), due to a smaller LW warming. Constrained by a global mean DAOD, model sensitivity studies of increasing horizontal and vertical resolution show strong influences on the simulated global dust burden and lifetime primarily through the change of dust dry deposition rate; there are also remarkable differences in simulated spatial distributions of DAOD, DRE, and deposition fluxes. Thus, constraining the global DAOD is insufficient for accurate representation of dust climate effects, especially in transitioning to higher- or variable-resolution ESMs. Better observational constraints of dust vertical profiles, dry deposition, size, and LW properties are needed.

54 ENVIRONMENTAL SCIENCES↗

Establishing robust correction schemes for improved and reliable ARM-AOS aerosol optical data products

Aerosol light absorption and scattering of solar radiation play an important role in the earth’s atmosphere in terms of direct and semi-direct radiative forcing. Optical parameters of importance to the US Department of Energy (DOE) climate models include absorption and scattering coefficients, single scattering albedo (SSA), absorption Angstrom exponents (AAE), and the asymmetry parameter (g). These parameters depend on aerosol size, shape and composition (refractive index), and are spectrally sensitive in the shortwave region. Additionally, these parameters have a complex dependency on the emission source, especially for carbonaceous aerosols. The DOE Atmospheric Radiation Measurement (ARM) user facility has deployed aerosol observing systems (AOS) containing several filter-based instruments to measure and constrain aerosol optical properties and related parameters at multiple sites worldwide. For measurement of aerosol light absorption, the AOS includes filter-based instruments (particle soot absorption photometer and tricolor absorption photometer) that infer particle-phase aerosol absorption coefficients at nominal red, green, and blue wavelength bands from the attenuation (ATN) of light passing through a particulate filter on which aerosols are deposited. Measurement of aerosol scattering is done in situ using nephelometers. By combining inferred absorption coefficients from filter-based ATN measurements and in situ scattering coefficients, value-added products (VAPs) such as SSA, AAE, and g are derived.

54 ENVIRONMENTAL SCIENCES↗

Improved Dust Representation and Impacts on Dust Transport and Radiative Effect in CAM5

Dust transport and spatial distribution are poorly represented in current global climate models (GCMs) including the Community Atmosphere Model version 5 (CAM5). Particularly, models lack explicit representation of super-coarse dust, which may have important implications for dust radiative forcing and impacts on biogeochemistry. A nine-mode version of the modal aerosol model (MAM9) has been developed to address these issues. In this new aerosol scheme, four dust modes have been designed to treat dust particles of sizes up to 20 μm. The MAM9-simulated results are compared with those from the default four-mode version of MAM (MAM4) and also with the in situ surface measurements of dust concentration and deposition flux, satellite-retrieved dust extinction profile, and in situ vertical measurements of dust concentrations from the NASA Atmosphere Tomography Mission (ATom). Overall, MAM9 improves the dust representation in remote regions while maintaining reasonably good results near the dust source regions. In addition, MAM9 reduces the fine dust burden and increases the coarse dust burden globally. The increased coarse dust burden has slightly increased the dust direct radiative effect by 0.01 W m –2 while it enhanced dust indirect radiative effect by 0.36 W m –2 , globally.

58 GEOSCIENCES↗