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At least 1,243 records · Page 69
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DOE OSTI2024

Broadband and filter radiometers at Ross Island, Antarctica: detection of cloud ice phase versus liquid water influences on shortwave and longwave radiation

Abstract. Surface radiometer data from Ross Island, Antarctica, collected during the austral summer 2015–2016 by the US Department of Energy Atmospheric Radiation Measurement (ARM) program West Antarctic Radiation Experiment (AWARE), are used to evaluate how shortwave and longwave irradiance respond to changing cloud properties as governed by contrasting meteorological regimes. Shortwave atmospheric transmittance is derived from pyranometer measurements, and cloud conservative-scattering optical depth is derived from filter radiometer measurements at 870 nm. With onshore flow associated with marine air masses, clouds contain mostly liquid water. With southerly flow over the Transantarctic Mountains, orographic forcing induces substantial cloud ice water content. These ice and mixed-phase clouds attenuate more surface shortwave irradiance than the maritime-influenced clouds and also emit less longwave irradiance due to colder cloud base temperature. These detected irradiance changes are in a range that can mean onset or inhibition of surface melt over ice shelves. This study demonstrates how basic and relatively low-cost broadband and filter radiometers can be used to detect subtle climatological influences of contrasting cloud microphysical properties at very remote locations.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Size-resolved process understanding of stratospheric sulfate aerosol following the Pinatubo eruption

Stratospheric sulfate aerosol produced by volcanic eruptions plays important roles in atmospheric chemistry and the global radiative balance of the atmosphere. The simulation of stratospheric sulfate concentrations and optical properties is highly dependent on the chemistry scheme and microphysical treatment. In this work, we implemented a sophisticated gas-phase chemistry scheme (full chemistry, FC) and a 5-mode version of the Modal Aerosol Module with Prognostic Stratospheric Aerosol (MAM5-PSA) for the interactive treatment of stratospheric sulfate aerosol in the Department of Energy's Energy Exascale Earth System Model version 2 (E3SMv2) model to better simulate the chemistry-aerosol feedback following the Pinatubo eruption, and to compare it against a simulation using simplified chemistry (SC) and the default 4-mode version of the Modal Aerosol Module (MAM4). MAM5-PSA experiments were found to better capture the stratospheric sulfate burden from the eruption of the volcano to the end of 1992 as compared to the High-resolution Infrared Sounder (HIRS) observations, and the formation of sulfate in MAM5-PSA with FC (with an additional OH replenishment reaction) was significantly faster than in MAM4 with FC. Analyses of microphysical processes indicate that more sulfate aerosol mass was generated in total in FC experiments than in SC experiments. MAM5-PSA performs better than MAM4 in simulation of aerosol optical depth (AOD); AOD anomalies from the MAM5-PSA experiment have better agreement with observations. The simulated largest changes in global mean net radiative flux at the top of the atmosphere following the eruption were about −3 W m −2 in MAM5-PSA experiments and roughly −1.5 W m −2 in MAM4 experiments.

AEROSOL↗
DOE OSTI2025

Technical note: Recommendations for diagnosing cloud feedbacks and rapid cloud adjustments using cloud radiative kernels

Abstract. The cloud radiative kernel method is a popular approach to quantify cloud feedbacks and rapid cloud adjustments to increased CO2 concentrations and to partition contributions from changes in cloud amount, altitude, and optical depth. However, because this method relies on cloud property histograms derived from passive satellite sensors or produced by passive satellite simulators in models, changes in obscuration of lower-level clouds by upper-level clouds can cause apparent low-cloud feedbacks and adjustments, even in the absence of changes in lower-level cloud properties. Here, we provide a methodology for properly diagnosing the impact of changing obscuration on cloud feedbacks and adjustments and quantify these effects across climate models. Averaged globally and across global climate models, properly accounting for obscuration leads to weaker positive feedbacks from lower-level clouds and stronger positive feedbacks from upper-level clouds while simultaneously removing a mostly artificial anti-correlation between them. Given that the methodology for diagnosing cloud feedbacks and adjustments using cloud radiative kernels has evolved over several papers, and obscuration effects have only occasionally been considered in recent papers, this paper serves to establish recommended best practices and to provide a corresponding code base for community use.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Remote-sensing detectability of airborne Arctic dust

Remote-sensing (RS)-based estimates of Arctic dust are oftentimes overestimated due to a failure in separating out the dust contribution from that of spatially homogeneous clouds or low-altitude cloud-like plumes. A variety of illustrations are given with a particular emphasis on questionable claims of using brightness temperature differences (BTDs) as a signature indicator of Arctic dust transported from mid-latitude deserts or generated by local Arctic sources. While there is little dispute about the presence of both Asian and local dust across the Arctic, the direct RS detectability of airborne dust, as ascribed to satellite (MODIS and AVHRR) measurements of significantly negative brightness temperature differences at 11 and 12 µm (BTD 11–12 ), has been misrepresented in certain cases. While it is difficult to account for all examples of strongly negative BTD 11–12 values in the Arctic, it is unlikely that airborne dust plays a significant role. One much more likely contributor would be water clouds in the Arctic inversion layer. The RS detectability of the impact of Arctic dust (notably due to Arctic dust from local sources) can, however, be of significance. Sustained dust deposition can substantially decrease (visible to shortwave IR) snow and ice reflectance albedo (pan-chromatic reflectance) and the signal measured by satellite sensors. Significantly negative BTD 11–12 values would, however, only represent a limited area near the drainage basin sources according to our event-level case studies. The enhanced ice-nucleating particle (INP) role of local Arctic dust can, for example, induce significant changes in the properties of low-level mixed-phase clouds (cloud optical depth changes <~ 1) that can readily be detected by active and passive RS instruments. It is critical that the distinction between the RS detectability of airborne Arctic dust versus the RS detectability of the impacts of that dust be understood if we are to appropriately parameterize, for example, the radiative forcing influence of dust in this climate-sensitive region.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Dust semi-direct effects: low-level cloud response to free-tropospheric dust-induced longwave radiation over the North Atlantic Ocean

Aerosol semi-direct effect is the adjustment of the radiative budget due to the cloud response to radiation absorption. Although dust accounts for about a third of aerosols' shortwave absorption, our understanding of its semi-direct effect often relies on traditional shortwave-focused mechanisms previously established for biomass-burning aerosols, and implications of dust longwave absorption on clouds have yet to be explored. Here, we assess the low-level cloud cover (LLCC) response to changes in properties and characteristics of the free-tropospheric dust layer over the North Atlantic Ocean (May–August, 2007–2017). We find that, consistent with previous studies, LLCC typically responds positively (increases in clouds) to an overlying dust layer. However, this response weakens with increasing dust optical depth (DOD), dust geometric thickness (DGT), and dust-layer base height (DBH). Specifically, we find that the LLCC response weakens by 4.3 ± 1.04 % and 1.6 ± 0.65 %, respectively, for a one-standard-deviation increase in DOD and DGT, and a smaller response to DBH (0.19 ± 0.45 %). We also find that the weakened LLCC response is primarily due to enhanced dust-induced longwave-dominated cloud-top warming, which counteracts the mean cloud-top cooling by as much as 19 % (mean of 9 %). Sensitivity analysis further indicates that the variability in dust properties, influenced by dust size distribution and refractive index, dominates the changes in dust-induced cloud-top warming, rather than variabilities in cloud properties or thermodynamic profiles. Our result adds to the traditional understanding of LLCC enhancement through shortwave-driven atmospheric stability, often associated with aerosol semi-direct effects, and highlights the role of dust-induced cloud-top longwave warming in dust semi-direct effects.

Pandey, Satyendra K. [Univ. of California, Merced,↗
DOE OSTI2026

Advancing the quantification of aerosol-cloud interactions with the CALIPSO-CloudSat-Aqua/MODIS record

Aerosol-cloud-precipitation interactions are assessed over the non-polar ocean using more than 11 years of combined Aqua-MODIS, CALIPSO-CALIOP, and CloudSat products. The analysis first shows the benefit of incorporating vertically resolved aerosol extinction coefficient (σext) in aerosol-cloud interactions (ACI) assessments, demonstrating that: σext vertically collocated with the cloud layer () correlates best with cloud droplet number concentration (Nd), column-integrated aerosol optical depth (AOD) cannot explain the Nd variability in the extratropics, and the S-shape of the AOD-Nd relationship reported in previous studies is not replicated when using instead of AOD, with a Nd- linearity more consistent with in-situ studies over the ocean. ACI metric, estimated as the log-scale regression between CALIOP and MODIS Nd reveals that the eastern Pacific is the region with the strongest ACI, followed by the Southern Ocean. The susceptibility of clouds to changes in their liquid water path (LWP) and frequency of precipitation followed a 2-step calculation by combining the Nd- regression (ACI) with the regression between these macrophysical variables and Nd. LWP susceptibility is negative (LWP decreases with aerosol loading) and statistically significant over the eastern Pacific, eastern Atlantic, and extratropics. In contrast, vast areas of the tropical and subtropical ocean feature negligible changes in LWP with aerosol. Precipitation frequency susceptibility is negative, but the values are only significant over the coastal eastern Pacific and Atlantic. The findings suggest that previous modeling assessments relying on AOD may need to be revisited by taking advantage of the synergy between passive and active sensors.

Li, Zhujun↗
DOE OSTI2023

Validation of the Cloud_CCI (Cloud Climate Change Initiative) cloud products in the Arctic

The role of clouds in the Arctic radiation budget is not well understood. Ground-based and airborne measurements provide valuable data to test and improve our understanding. However, the ground-based measurements are intrinsically sparse, and the airborne observations are snapshots in time and space. Passive remote sensing measurements from satellite sensors offer high spatial coverage and an evolving time series, having lengths potentially of decades. However, detecting clouds by passive satellite remote sensing sensors is challenging over the Arctic because of the brightness of snow and ice in the ultraviolet and visible spectral regions and because of the small brightness temperature contrast to the surface. Consequently, the quality of the resulting cloud data products needs to be assessed quantitatively. In this study, we validate the cloud data products retrieved from the Advanced Very High Resolution Radiometer (AVHRR) post meridiem (PM) data from the polar-orbiting NOAA-19 satellite and compare them with those derived from the ground-based instruments during the sunlit months. The AVHRR cloud data products by the European Space Agency (ESA) Cloud Climate Change Initiative (Cloud_CCI) project uses the observations in the visible and IR bands to determine cloud properties. The ground-based measurements from four high-latitude sites have been selected for this investigation: Hyytiälä (61.84°N, 24.29°E), North Slope of Alaska (NSA; 71.32°N, 156.61°W), Ny-Ålesund (Ny-Å; 78.92°N, 11.93°E), and Summit (72.59°N, 38.42°W). The liquid water path (LWP) ground-based data are retrieved from microwave radiometers, while the cloud top height (CTH) has been determined from the integrated lidar–radar measurements. The quality of the satellite products, cloud mask and cloud optical depth (COD), has been assessed using data from NSA, whereas LWP and CTH have been investigated over Hyytiälä, NSA, Ny-Å, and Summit.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Evaluation of four ground-based retrievals of cloud droplet number concentration in marine stratocumulus with aircraft in situ measurements

Abstract. Cloud droplet number concentration (Nd) is crucial for understanding aerosol–cloud interactions (ACI) and associated radiative effects. We present evaluations of four ground-based Nd retrievals based on comprehensive datasets from the Atmospheric Radiation Measurement (ARM) Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign. The Nd retrieval methods use ARM ENA observatory ground-based remote sensing observations from a micropulse lidar, Raman lidar, cloud radar, and the ARM NDROP (Droplet Number Concentration) value-added product (VAP), all of which also retrieve cloud effective radius (re). The retrievals are compared against aircraft measurements from the fast cloud droplet probe (FCDP) and the cloud and aerosol spectrometer (CAS) obtained from low-level marine boundary layer clouds on 12 flight days during summer and winter seasons. Additionally, the in situ measurements are used to validate the assumptions and characterizations used in the retrieval algorithms. Statistical comparisons of the probability distribution function (PDF) of the Nd and cloud re retrievals with aircraft measurements demonstrate that these retrievals align well with in situ measurements for overcast clouds, but they may substantially differ for broken clouds or clouds with low liquid water path (LWP). The retrievals are applied to 4 years of ground-based remote sensing measurements of overcast marine boundary layer clouds at the ARM ENA observatory to find that Nd (re) values exhibit seasonal variations, with higher (lower) values during the summer season and lower (higher) values during the winter season. The ensemble of various retrievals using different measurements and retrieval algorithms such as those in this paper can help to quantify Nd retrieval uncertainties and identify reliable Nd retrieval scenarios. Of the retrieval methods, we recommend using the micropulse lidar-based method. This method has good agreement with in situ measurements, less sensitivity to issues arising from precipitation and low cloud LWP and/or optical depth, and broad applicability by functioning for both daytime and nighttime conditions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Evaluation of the hyperspectral radiometer (HSR1) at the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site

Abstract. The Peak Design Ltd hyperspectral radiometer (HSR1) was tested at the Atmospheric Radiation Measurement (ARM) user facility Southern Great Plains (SGP) site in Lamont, Oklahoma, for 2 months from May to July 2022. The HSR1 is a prototype instrument that measures total (Ftotal) and diffuse (Fdiffuse) spectral irradiance from 360 to 1100 nm with a spectral resolution of 3 nm. The HSR1 spectral irradiance measurements are compared to nearby collocated spectral radiometers, including two multifilter rotating shadowband radiometers (MFRSRs) and the Shortwave Array Spectroradiometer–Hemispheric (SASHe) radiometer. The Ftotal at 500 nm for the HSR1 compared to the MFRSRs has a mean (relative) difference of 0.01 W m−2 nm−1 (1 %–2 %). The HSR1 mean Fdiffuse at 500 nm is smaller than the MFRSRs' by 0.03–0.04 (10 %) W m−2 nm−1. The HSR1 clear-sky aerosol optical depth (AOD) is also retrieved by considering Langley regressions and compared to collocated instruments such as the Cimel sunphotometer (CSPHOT), MFRSRs, and SASHe. The mean HSR1 AOD at 500 nm is larger than the CSPHOT's by 0.010 (8 %) and larger than the MFRSRs' by 0.007–0.017 (6 %–18 %). In general, good agreement between the HSR1 and other instruments is found in terms of the Ftotal, Fdiffuse, and AODs at 500 nm. The HSR1 quantities are also compared at other wavelengths to the collocated instruments. The comparisons are within ∼ 10 % for the Ftotal and Fdiffuse, except for 940 nm, where there is relatively larger disagreement. The AOD comparisons are within ∼ 10 % at 415 and 440 nm; however, a relatively larger disagreement in the AOD comparison is found for higher wavelengths.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Marine and continental stratocumulus cloud microphysical properties obtained from routine ARM Cimel sunphotometer observations

This study investigates marine and continental stratocumulus (Sc) cloud properties obtained from an automated implementation of a multispectral photometer retrieval. Photometer methods simultaneously retrieve cloud optical depth (τ) and cloud droplet effective radius (r e ), with estimates for liquid water path (LWP) calculated on the availability of those quantities. These applied methods evaluate retrieved cloud properties for Sc identified during a recent 6 year period over the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) program sites in Oklahoma, USA (SGP) and in the Azores, Portugal (ENA). Modest agreement in key quantity retrievals is found between the routine photometer products and multisensor collocated profiling references. Cumulative breakdowns contingent on cloud thickness indicate increases in all retrieved quantities in thicker clouds, with larger discrepancies in the relative performance between the retrievals collected in the presence of drizzle. Under continental cloud conditions, the clouds of a similar thickness and r e to those sampled under marine conditions report a factor of 1.5 larger τ and LWP. An r 2 ≅0.65 is found between photometer τ retrievals and shadowband radiometer measurements, with photometer retrievals reporting a high (relative) bias. The τ intercomparisons indicate that variability between retrievals is a factor of three larger than errors reported from individual retrieval input perturbation tests. Photometer r e retrievals suggest a low r 2 (< 0.1) having a standard deviation ≅ 3 µm when compared to ARM baseline multi-sensor radar/radiometer references (accounting for offsets in the cloud droplet number concentration assumptions of the latter). However, photometer LWP calculations remain relatively unbiased in non-drizzling conditions, with errors O (50 g m −2 ) and r 2 ≅0.5 to collocated radiometer and interferometer references. Additional sensitivity tests for island influences on marine Sc properties suggest that while island-influenced winds may promote larger cloud LWP or thickness, the influence could be within retrieval method uncertainty and/or collocated instrument variability.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Leveraging machine learning to enhance aerosol classification using Single-Particle Mass Spectrometry

Advancing automated classification of atmospheric aerosols from Single-Particle Mass Spectrometry (SPMS) data remains challenging due to overlapping ion signatures, compositional diversity, and limited labeled data. This study evaluates supervised and semi-supervised learning frameworks to enhance aerosol identification by jointly leveraging labeled and unlabeled spectra. Four models were compared: a supervised Support Vector Machine (SVM), a self-training SVM, a stacked autoencoder classifier, and a stacked autoencoder trained using a temporal-ensembling Mean Teacher approach. All models achieved high and stable accuracies (90.0 %–91.1 %), surpassing previous results on the same dataset (87 %) and matching the performance of state-of-the-art deep learning methods. Despite small global metric differences (≤ 1 %), semi-supervised variants yielded up to 5 %–10 % improvements for compositionally rare particle types – such as soot (0.77 % of spectra, F1-score: 0.93–0.97) and hazelnut pollen (0.98 % of spectra, F1-score: 0.97–1.00) – equating to roughly ∼ 187 additional correctly classified spectra. These gains are scientifically significant, as such rare particles exert disproportionate influence on radiative absorption and ice nucleation processes; their improved detection reduces modeled uncertainties in aerosol absorption optical depth and mixed-phase cloud ice nucleation rates. The models' residual misclassifications (≈ 9 %) largely arise from true spectral overlap among chemically adjacent species (e.g., Na- vs. K-feldspar, coated vs. uncoated feldspars), reflecting physical compositional continuity rather than algorithmic error. Collectively, these findings demonstrate that leveraging unlabeled data to learn robust spectral representations and refine classification enhances both fidelity and interpretability, bridging data-driven analysis with aerosol–climate process understanding.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Hemispherically symmetric strategies for stratospheric aerosol injection

Stratospheric aerosol injection (SAI) comes with a wide range of possible design choices, such as the location and timing of the injection. Different stratospheric aerosol injection strategies can yield different climate responses; therefore, understanding the range of possible climate outcomes is crucial to making informed future decisions on SAI, along with the consideration of other factors. Yet, to date, there has been no systematic exploration of a broad range of SAI strategies. This limits the ability to determine which effects are robust across different strategies and which depend on specific injection choices. This study systematically explores how the choice of SAI strategy affects climate responses in one climate model. Here, we introduce four hemispherically symmetric injection strategies, all of which are designed to maintain the same global mean surface temperature: an annual injection at the Equator (EQ), an annual injection of equal amounts of SO 2 at 15° N and 15° S (15N+15S), an annual injection of equal amounts of SO 2 at 30° N and 30° S (30N+30S), and a polar injection strategy that injects equal amounts of SO 2 at 60° N and 60° S only during spring in each hemisphere (60N+60S). We compare these four hemispherically symmetric SAI strategies with a more complex injection strategy that injects different quantities of SO 2 at 30° N, 15° N, 15° S, and 30° S in order to maintain not only the global mean surface temperature but also its large-scale horizontal gradients. All five strategies are simulated using version 2 of the Community Earth System Model with the middle atmosphere version of the Whole Atmosphere Community Climate model, version 6, as the atmospheric component, CESM2(WACCM6-MA), with the global warming scenario, Shared Socioeconomic Pathway (SSP)2-4.5. We find that the choice of SAI strategy affects the spatial distribution of aerosol optical depths, injection efficiency, and various surface climate responses. In addition, injecting in the subtropics produces more global cooling per unit injection, with the EQ and the 60N+60S cases requiring, respectively, 59 % and 50 % more injection than the 30N+30S case to meet the same global mean temperature target. Injecting at higher latitudes results in larger Equator-to-pole temperature gradients. While all five strategies restore Arctic September sea ice, the high-latitude injection strategy is more effective due to the SAI-induced cooling occurring preferentially at higher latitudes. These results suggest trade-offs wherein different strategies appear better or worse, depending on which metrics are deemed important.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

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↗
DOE OSTI2026

Subsets of geostationary satellite data over international observing network sites for studying the diurnal dynamics of energy, carbon, and water cycles

The latest generation of geostationary satellites provide Earth observations similar to widely used polar-orbiting sensors but at intervals as frequently as every 5–10 min, making them ideal for studying the diurnal dynamics of land–atmosphere interactions. The NASA Earth Exchange (NEX) group created the GeoNEX datasets by collating data from several geostationary platforms, including GOES-16/17/18, Himawari-8/9, and GK-2A, and placing them on a common grid to facilitate use by the Earth science community. Here, we document the GeoNEX Coincident Ground Observations (GeCGO) dataset for terrestrial ecosystem studies and provide examples for its use. Currently, GeCGO provides GOES-16 Advanced Baseline Imager (ABI) data over a 10 km × 10 km area surrounding 1586 network sites across the Americas. GeCGO makes it easy to compare the time series of geostationary data with the diurnal ground observations, including carbon/water fluxes and aerosol optical depth, and is extensible to other regions. We also develop GeoNEXTools to facilitate analyses that require both GeoNEX data and other NASA satellite data. The objectives of this paper are to introduce GeCGO and GeoNEXTools and demonstrate their applications. First, we describe the details of GeCGO and GeoNEXTools. Second, we explain how GeCGO can be integrated with other satellite data. Finally, we showcase comparisons between GeCGO and observations from three ground-based networks. GeCGO is available at https://doi.org/10.25966/y5pe-xp41 (Hashimoto et al., 2025).

Hashimoto, Hirofumi [NASA Ames Research Center (AR↗
DOE OSTI2023

Towards an improved representation of carbonaceous aerosols over the Indian monsoon region in a regional climate model: RegCM

Mitigation of carbonaceous aerosol emissions is expected to provide climate and health co-benefits. The accurate representation of carbonaceous aerosols in climate models is critical for reducing uncertainties in their climate feedback. In this regard, emission fluxes and aerosol life cycle processes are the two primary sources of uncertainties. Here, we demonstrate that the incorporation of a dynamic ageing scheme and emission estimates that are updated for the local sources improves the representation of carbonaceous aerosols over the Indian monsoon region in a regional climate model, RegCM, compared with its default configuration. The respective mean black carbon (BC) and organic carbon (OC) surface concentrations in 2010 are estimated to be 4.25 and 10.35 µg m -3 over the Indo-Gangetic Plain (IGP) in the augmented model. The BC column burden over the polluted IGP is found to be 2.47 mg m -2 , 69.95 % higher than in the default model configuration and much closer to available observations. The anthropogenic aerosol optical depth (AOD) increases by more than 19 % over the IGP due to the model enhancement, also leading to a better agreement with observed AOD. The respective top-of-the-atmosphere, surface, and atmospheric anthropogenic aerosol short-wave radiative forcing are estimated at -0.3, -9.3, and 9.0 W m -2 over the IGP and -0.89, -5.33, and 4.44 W m -2 over Peninsular India (PI). Our results suggest that the combined effect of two modifications leads to maximum improvements in the model performance in regions where emissions play a dominant role.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Assessing the sensitivity of aerosol mass budget and effective radiative forcing to horizontal grid spacing in E3SMv1 using a regional refinement approach

Abstract. Atmospheric aerosols have important impacts on air quality and the Earth–atmospheric energy balance. However, as computing power is limited, Earth system models generally use coarse spatial grids and parameterize finer-scale atmospheric processes. These parameterizations and the simulation of atmospheric aerosols are often sensitive to model horizontal resolutions. Understanding the sensitivities is necessary for the development of Earth system models at higher resolutions with the deployment of more powerful supercomputers. Using the Energy Exascale Earth System Model (E3SM) version 1, this study investigates the impact of horizontal grid spacing on the simulated aerosol mass budget, aerosol–cloud interactions, and the effective radiative forcing of anthropogenic aerosols (ERFaer) over the contiguous United States. We examine the resolution sensitivity by comparing the nudged simulation results for 2016 from the low-resolution model (LR) and the regional refinement model (RRM). As expected, the simulated emissions of natural dust, sea salt, and marine organic matter are substantially higher in the RRM than in the LR. In addition, RRM simulates stronger aqueous-phase production of sulfate through the enhanced oxidation of sulfur dioxide by hydrogen peroxide due to increased cloud liquid water content. In contrast, the gas-phase chemical production of sulfate is slightly suppressed. The RRM resolves more large-scale precipitation and produces less convective precipitation than the LR, leading to increased (decreased) aerosol wet scavenging by large-scale (convective) precipitation. Regarding aerosol effects on clouds, RRM produces larger temporal variabilities in the large-scale liquid cloud fractions than LR, resulting in increased microphysical cloud processing of aerosols (more interstitial aerosols are converted to cloud-borne aerosols via aerosol activation) in RRM. Water vapor condensation is also enhanced in RRM compared to LR. Consequently, the RRM simulation produces more cloud droplets, a larger cloud droplet radius, a higher liquid water path, and a larger cloud optical depth than the LR simulation. A comparison of the present-day and pre-industrial simulations indicates that, for this contiguous United States domain, the higher-resolution increases ERFaer at the top of the model by about 12 %, which is mainly attributed to the strengthened indirect effect associated with aerosol–cloud interactions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Impacts of spatial heterogeneity of anthropogenic aerosol emissions in a regionally refined global aerosol–climate model

Abstract. Emissions of anthropogenic aerosol and their precursors are often prescribed in global aerosol models. Most of these emissions are spatially heterogeneous at model grid scales. When remapped from low-resolution data, the spatial heterogeneity in emissions can be lost, leading to large errors in the simulation. It can also cause the conservation problem if non-conservative remapping is used. The default anthropogenic emission treatment in the Energy Exascale Earth System Model (E3SM) is subject to both problems. In this study, we introduce a revised emission treatment for the E3SM Atmosphere Model (EAM) that ensures conservation of mass fluxes and preserves the original emission heterogeneity at the model-resolved grid scale. We assess the error estimates associated with the default emission treatment and the impact of improved heterogeneity and mass conservation in both globally uniform standard-resolution (∼ 165 km) and regionally refined high-resolution (∼ 42 km) simulations. The default treatment incurs significant errors near the surface, particularly over sharp emission gradient zones. Much larger errors are observed in high-resolution simulations. It substantially underestimates the aerosol burden, surface concentration, and aerosol sources over highly polluted regions, while it overestimates these quantities over less-polluted adjacent areas. Large errors can persist at higher elevation for daily mean estimates, which can affect aerosol extinction profiles and aerosol optical depth (AOD). We find that the revised treatment significantly improves the accuracy of the aerosol emissions from surface and elevated sources near sharp spatial gradient regions, with significant improvement in the spatial heterogeneity and variability of simulated surface concentration in high-resolution simulations. In the next-generation E3SM running at convection-permitting scales where the resolved spatial heterogeneity is significantly increased, the revised emission treatment is expected to better represent the aerosol emissions as well as their lifecycle and impacts on climate.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

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)↗