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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Characteristics and effects of aerosols during blowing snow events in the central Arctic

Sea salt aerosol (SSaer) significantly impacts aerosol-radiation and aerosol-cloud interactions, and sublimated blowing snow is hypothesized to be an important SSaer source in polar regions. Understanding blowing snow and other wind-sourced aerosols’ climate relevant properties is needed, especially during winter when Arctic amplification is greatest. However, most of our understanding of blowing snow SSaer comes from modeling studies, and direct observations are sparse. Additionally, SSaer can originate from multiple sources, making it difficult to disentangle emission processes. Here, we present comprehensive observations of wind-sourced aerosol during blowing snow events from the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition in the central Arctic. High wind speed strongly enhances total aerosol number, submicron sodium chloride mass, cloud condensation nuclei concentrations, and scattering coefficients. Generally, the relative response of aerosol properties to wind speed enhancement is strongest in fall when Arctic aerosol concentrations are lowest. Blowing snow events showed similar aerosol and environmental properties across events, apart from occasions with high snow age (>6 days since last snowfall). Coarse-mode number concentrations (>1 μm) are better explained by variability in wind speed averaged over 12-h air mass back trajectories arriving at the MOSAiC site compared to local, instantaneous wind speed, suggesting the importance of regional transport and consideration of air mass history for wind-driven aerosol production. These MOSAiC observations provide new insights into wind-driven aerosol in the central Arctic and may help validate modeling studies and improve model parameterizations particularly for aerosol direct and indirect radiative forcing.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Bounding Global Aerosol Radiative Forcing of Climate Change

Abstract Aerosols interact with radiation and clouds. Substantial progress made over the past 40 years in observing, understanding, and modeling these processes helped quantify the imbalance in the Earth's radiation budget caused by anthropogenic aerosols, called aerosol radiative forcing, but uncertainties remain large. This review provides a new range of aerosol radiative forcing over the industrial era based on multiple, traceable, and arguable lines of evidence, including modeling approaches, theoretical considerations, and observations. Improved understanding of aerosol absorption and the causes of trends in surface radiative fluxes constrain the forcing from aerosol‐radiation interactions. A robust theoretical foundation and convincing evidence constrain the forcing caused by aerosol‐driven increases in liquid cloud droplet number concentration. However, the influence of anthropogenic aerosols on cloud liquid water content and cloud fraction is less clear, and the influence on mixed‐phase and ice clouds remains poorly constrained. Observed changes in surface temperature and radiative fluxes provide additional constraints. These multiple lines of evidence lead to a 68% confidence interval for the total aerosol effective radiative forcing of ‐1.6 to ‐0.6 W m −2 , or ‐2.0 to ‐0.4 W m −2 with a 90% likelihood. Those intervals are of similar width to the last Intergovernmental Panel on Climate Change assessment but shifted toward more negative values. The uncertainty will narrow in the future by continuing to critically combine multiple lines of evidence, especially those addressing industrial‐era changes in aerosol sources and aerosol effects on liquid cloud amount and on ice clouds.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Aitken Mode Aerosols Buffer Decoupled Mid‐Latitude Boundary Layer Clouds Against Precipitation Depletion

Aerosol-cloud-precipitation interactions are a leading source of uncertainty in estimating climate sensitivity. Remote marine boundary layers where accumulation mode (~100–400 nm diameter) aerosol concentrations are relatively low are very susceptible to aerosol changes. These regions also experience heightened Aitken mode aerosol (~10–100 nm) concentrations associated with ocean biology. Aitken aerosols may significantly influence cloud properties and evolution by replenishing cloud condensation nuclei and droplet number lost through precipitation (i.e., Aitken buffering). We use a large-eddy simulation with an Aitken-mode enabled microphysics scheme to examine the role of Aitken buffering in a mid-latitude decoupled boundary layer cloud regime observed on 15 July 2017 during the Aerosol and Cloud Experiments in the Eastern North Atlantic flight campaign: cumulus rising into stratocumulus under elevated Aitken concentrations (~100–200 mg -1 ). In situ measurements are used to constrain and evaluate this case study. Our simulation accurately captures observed aerosol-cloud-precipitation interactions and reveals time-evolving processes driving regime development and evolution. Aitken activation into the accumulation mode in the cumulus layer provides a reservoir for turbulence and convection to carry accumulation aerosols into the drizzling stratocumulus layer above. Further Aitken activation occurs aloft in the stratocumulus layer. Together, these activation events buffer this cloud regime against precipitation removal, reducing cloud break-up and associated increases in heterogeneity. We examine cloud evolution sensitivity to initial aerosol conditions. With halved accumulation number, Aitken aerosols restore accumulation concentrations, maintain droplet number similar to original values, and prevent cloud break-up. Without Aitken aerosols, precipitation-driven cloud break-up occurs rapidly. In this regime, Aitken buffering sustains brighter, more homogeneous clouds for longer.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

All-sky aerosol direct radiative effects at the ARM SGP site

All-sky aerosol direct radiative effect (DRE) was estimated for the first time at the Atmospheric Radiation Measurement Southern Great Plains site using multi-year ground-based observations. The NASA Langley Fu-Liou radiation model was employed. Observed inputs for the radiation model include aerosol and cloud vertical extinction profile from Raman lidar; spectral aerosol optical depth, single-scattering albedo, and asymmetry factor from Aerosol Robotic Network; cloud water content profiles from radars; temperature and water vapor profiles from radiosondes; and surface shortwave spectral albedo from radiometers. A cloudy-sky radiative closure experiment was performed. The relative mean differences between modeled and observed surface downwelling shortwave total fluxes were 6% (7%) for transparent (opaque) cloudy-skies. The estimated annual mean all-sky aerosol DRE is -2.13±0.54W m -2 at the top of atmosphere (TOA) and -5.95±0.87 W m -2 at the surface, compared to -3.00±0.58 W m -2 AND -6.85±1.00 W m -2 , respectively, under clear-sky conditions. The seasonal cycle of all-sky aerosol DRE is similar to that of the clear-sky, except with secondary influences of the clouds: The cloud radiative effect is strongest (most negative) in the spring, which reduces the all-sky aerosol DRE. The relative uncertainties in all-sky aerosol DRE due to measurement errors are generally comparable to those in clear-sky conditions except for the aerosol single-scattering albedo. Finally, the TOA all-sky aerosol DRE relative uncertainty due to aerosol single-scattering albedo uncertainty is larger than that in clear-sky, leading to a larger total relative uncertainty. The measurement errors in cloud properties have small effects on the all-sky aerosol DRE.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Pluminate: Quantifying aerosol injection behavior from simulation, experimentation and observations

Marine aerosol injections are a key component in further understanding of both the potentials of deliberate injection for marine cloud brightening (MCB), a potential climate intervention (CI) strategy, and key aerosol-cloud interaction behaviors that currently form the largest uncertainty in global climate model (GCM) predictions of our climate. Since the rate of spread of aerosols in a marine environment directly translates to the effectiveness and ability of aerosol injections in impacting cloud radiative forcing, it is crucial to understand the spatial and temporal extent of injected-aerosol effects following direct injection into marine environments. The ubiquity of ship-injected aerosol tracks from satellite imagery renders observational validation of new parameterizations possible in 2D, however, 3D compatible data is more scarce, and necessary for the development of subgrid scale parameterizations of aerosol-cloud interactions in GCMs. This report introduces two novel parameterizations of atmospheric aerosol injection behavior suitable for both 3D (GCM-compatible) and 2D (observation-related) modeling. Their applicability is highlighted using a wealth of different observational data: small and larger scale salt-aerosol injection experiments conducted at SNL, 3D large eddy simulations of ship-injected aerosol tracks and 2D satellite images of ship tracks. The power of experimental data in enhancing knowledge of aerosol-cloud interactions is in particular emphasized by studying key aerosol microphysical and optical properties as observed through their mixing in cloud-like environments.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Measurements and Analyses to Enable Science for the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE)

Coastal cities provide the opportunity to characterize the substantial effects of manmade particles on marine cloud properties and processes. La Jolla lies to the north of San Diego, California, but it is often about a day directly downwind of the major pollution sources located in the ports of Los Angeles and Long Beach. The large dynamic range of aerosol particle concentrations combined with the multi-hour to multi-day persistence of stratocumulus cloud layers makes the site ideal for investigating the seasonal changes in cloud and aerosol properties as well as the quantitative relationships between cloud and aerosol properties. The Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE) characterized the extent, radiative properties, aerosol interactions, and precipitation characteristics of stratocumulus clouds in the Eastern Pacific across all four seasons at two coastal sites in La Jolla. This project was designed to enhance and expand the scientific uses of the ARM AMF1 measurements from EPCAPE. The goal was to ensure meaningful observations were collected that would enable science. The project included the following objectives: (1) Reviewing the ARM AMF1 measurements [ARM, 2021a; b] and circulating a summary of the measurements each week, (2) Comparing AMF1 measurements to those provided by collaborators (including filter measurements at the pier), (3) Collecting and analyzing filter samples from Scripps Pier by Fourier Transform Infrared spectroscopy (FTIR) and X-ray Fluorescence (XRF), (4) Assisting in operations of instruments provided by Guest PIs when possible, and (5) Providing an initial compilation of EPCAPE aerosol and cloud seasonal differences. The expected outcomes of these objectives were enhanced proposals and publications using EPCAPE measurements by helping to identify instrument issues, expanded data access and awareness by distributing weekly plots and related summaries, improved source-related attribution of aerosols with elemental tracers, additional observations provided by Guest PIs, and accelerated ACI studies enabled by the compiled seasonal summaries of aerosol and cloud properties. Three examples of the science enabled by this project are findings that (i) aerosol and cloud aqueous production contributes more than half of sulfate particle mass concentration, (ii) upwind sources make chemical composition very similar at nearby sites despite local differences in meteorology, and (iii) most of the large mass concentration of semi-volatile organic components is co-emitted and co-evaporated with nitrate. Together these findings illustrate how ARM extended field campaigns in coastal regions can be used to constrain ACI processes with direct observations. By using the unique ARM suite of cloud radiative products in addition to the measured aerosol properties at a coastal location, we were able to address the more specific question of which aerosol particles cause how much of the effects on clouds. Identifying this signature in coastal areas provides an opportunity to test the representation of aerosol sources by global models in a range of clean and urban-influenced conditions.

Russell, Lynn [Univ. of California, San Diego, CA ↗
DOE OSTI2025

Real-Time Characterization of Salt Aerosols Generated from Static and Sparged Molten Salt

The formation of radionuclide-bearing aerosols in the respirable size range has the potential to significantly influence offsite dose consequences and is, therefore, an important consideration in nuclear facility safety assessments. Molten salt reactor (MSR) developers will likely need to demonstrate an understanding of the conditions under which radionuclide-bearing aerosols may be generated from their reactor under normal operating and accident conditions, as well as the characteristics and transport behavior of these aerosols, to demonstrate to the U.S. Nuclear Regulatory Commission (NRC) that the facility can be operated safely. Recent reviews of the literature identified a lack of experimental data describing the mechanisms of formation and properties (size, concentration, and composition) of salt aerosol particles that are produced from molten salts. Experiments that identify the conditions that lead to radionuclide-bearing salt aerosol releases and quantify the characteristics of salt aerosols formed by different mechanisms are high-priority needs to support MSR licensing. This report describes tests that were conducted within the Argonne Salt Aerosol Test Stand (a sealed vessel and measurement system) to generate salt aerosols from static and sparged molten salts and measure their size and concentration in real-time. The results provide insight into salt aerosol formation by the vapor condensation and bubble bursting mechanisms and inform the potential radiological consequences of aerosol formation from molten fuel salt. Videos of the salt surface were taken during salt sparge tests to observe surface bubble behavior. The data in this report can be used to develop mechanistic source term and accident progression models for MSRs. The real-time salt aerosol characterization technique used in this study will be employed in future integral effects tests that are conducted at an engineering scale to simulate realistic MSR accidents and in future separate effects tests to address additional variables that may impact salt aerosol characteristics (e.g., presence of fission products in salt and humidity in atmosphere).

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2020

Understanding and improving model representation of aerosol optical properties for a Chinese haze event measured during KORUS-AQ

KORUS-AQ was an international cooperative air quality field study in South Korea that measured local and remote sources of air pollution affecting the Korean Peninsula during May–June 2016. Some of the largest aerosol mass concentrations were measured during a Chinese haze transport event (24 May). Air quality forecasts using the WRF-Chem model with aerosol optical depth (AOD) data assimilation captured AOD during this pollution episode but overpredicted surface particulate matter concentrations in South Korea, especially PM 2.5 , often by a factor of 2 or larger. Analysis revealed multiple sources of model deficiency related to the calculation of optical properties from aerosol mass that explain these discrepancies. Using in situ observations of aerosol size and composition as inputs to the optical properties calculations showed that using a low-resolution size bin representation (four bins) underestimates the efficiency with which aerosols scatter and absorb light (mass extinction efficiency). Besides using finer-resolution size bins (8–16 bins), it was also necessary to increase the refractive indices and hygroscopicity of select aerosol species within the range of values reported in the literature to achieve better consistency with measured values of the mass extinction efficiency (6.7 m 2 g –1 observed average) and light-scattering enhancement factor (ƒ(RH)) due to aerosol hygroscopic growth (2.2 observed average). Furthermore, an evaluation of the optical properties obtained using modeled aerosol properties revealed the inability of sectional and modal aerosol representations in WRF-Chem to properly reproduce the observed size distribution, with the models displaying a much wider accumulation mode. Other model deficiencies included an underestimate of organic aerosol density (1.0 g cm –3 in the model vs. observed average of 1.5 g cm –3 ) and an overprediction of the fractional contribution of submicron inorganic aerosols other than sulfate, ammonium, nitrate, chloride, and sodium corresponding to mostly dust (17 %–28 % modeled vs. 12 % estimated from observations). These results illustrate the complexity of achieving an accurate model representation of optical properties and provide potential solutions that are relevant to multiple disciplines and applications such as air quality forecasts, health impact assessments, climate projections, solar power forecasts, and aerosol data assimilation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

The mechanisms and seasonal differences of the impact of aerosols on daytime surface urban heat island effect

The urban heat island intensity (UHII) is the temperature difference between urban areas and their rural surroundings. It is commonly attributed to changes in the underlying surface structure caused by urbanization. Air pollution caused by aerosol particles can affect the UHII through changing (1) the surface energy balance by the aerosol radiative effect (ARE) and (2) planetary-boundary-layer (PBL) stability and airflow intensity by modifying thermodynamic structure, which is referred to as the aerosol dynamic effect (ADE). By analyzing satellite data and ground-based observations collected from 2001 to 2010 at 35 cities in China and using the WRF-Chem model, we find that the impact of aerosols on UHII differs considerably: reducing the UHII in summer but increasing the UHII in winter. This seasonal contrast is proposed to be caused by the different strengths of the ARE and ADE between summer and winter. In summer, the ARE on UHII is dominant over the ADE, cooling down surface temperature more strongly in urban areas than in rural areas because of much higher aerosol loading, and offsets the urban heating, therefore weakening UHII. In winter, however, the ADE is more dominant, because aerosols stabilize the PBL more in the polluted condition, weakening the near-surface heat transport over urban areas in both vertical and horizontal directions. This means that the heat accumulated in urban areas is dispersed less effectively, and thus the UHII is enhanced. These findings shed new light on the impact of the interaction between urbanization-induced surface changes and air pollution on urban climate.urban areas and their rural surroundings. It is commonly attributed to changes in the underlying surface structure caused by urbanization. Air pollution caused by aerosol particles can affect the UHII through changing (1) the surface energy balance by the aerosol radiative effect (ARE) and (2) planetary-boundary-layer (PBL) stability and airflow intensity by modifying thermodynamic structure, which is referred to as the aerosol dynamic effect (ADE). By analyzing satellite data and ground-based observations collected from 2001 to 2010 at 35 cities in China and using the WRF-Chem model, we find that the impact of aerosols on UHII differs considerably: reducing the UHII in summer but increasing the UHII in winter. This seasonal contrast is proposed to be caused by the different strengths of the ARE and ADE between summer and winter. In summer, the ARE on UHII is dominant over the ADE, cooling down surface temperature more strongly in urban areas than in rural areas because of much higher aerosol loading, and offsets the urban heating, therefore weakening UHII. In winter, however, the ADE is more dominant, because aerosols stabilize the PBL more in the polluted condition, weakening the near-surface heat transport over urban areas in both vertical and horizontal directions. This means that the heat accumulated in urban areas is dispersed less effectively, and thus the UHII is enhanced. These findings shed new light on the impact of the interaction between urbanization-induced surface changes and air pollution on urban climate.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Aircraft measurements of aerosol and trace gas chemistry in the eastern North Atlantic

The Aerosol and Cloud Experiment in the Eastern North Atlantic (ACE-ENA) investigated properties of aerosols and subtropical marine boundary layer (MBL) clouds. Low subtropical marine clouds can have a large effect on Earth's radiative budget, but they are poorly represented in global climate models. In order to understand their radiative effects, it is imperative to understand the composition and sources of the MBL cloud condensation nuclei (CCN). The campaign consisted of two intensive operation periods (IOPs) (June–July 2017 and January–February 2018) during which an instrumented G-1 aircraft was deployed from Lajes Field on Terceira Island in the Azores, Portugal. The G-1 conducted research flights in the vicinity of the Atmospheric Radiation Measurement (ARM) Eastern North Atlantic (ENA) atmospheric observatory on Graciosa Island. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and Ionicon proton-transfer-reaction mass spectrometer (PTR-MS) were deployed aboard the aircraft, characterizing chemistry of non-refractory aerosol and trace gases, respectively. The eastern North Atlantic region was found to be very clean, with an average non-refractory submicrometer aerosol mass loading of 0.6 µg m −3 in the summer and 0.1 µg m −3 in the winter, measured by the AMS. Average concentrations of the trace reactive gases methanol and acetone were 1–2 ppb; benzene, toluene and isoprene were even lower, <1 ppb. Mass fractions of sulfate, organics, ammonium and nitrate in the boundary layer were 69 %, 23 %, 7 % and 1 % and remained largely similar between seasons. The aerosol chemical composition was dominated by sulfate and highly processed organics. Particulate methanesulfonic acid (MSA), a well-known secondary biogenic marine species, was detected, with an average boundary layer concentration of 0.021 µg m −3 , along with its gas-phase precursor, dimethyl sulfide (DMS). MSA accounted for no more than 3 % of the submicron, non-refractory aerosol in the boundary layer. Examination of vertical profiles of aerosol and gas chemistry during ACE-ENA reveals an interplay of local marine emissions and long-range-transported aged aerosol. A case of transport of biomass burning emissions from North American fires has been identified using back-trajectory analysis. In the summer, the non-refractory portion of the background CCN budget was heavily influenced by aerosol associated with ocean productivity, in particular sulfate formed from DMS oxidation. Episodic transport from the continents, particularly of biomass burning aerosol, periodically increased CCN concentrations in the free troposphere. In the winter, with ocean productivity lower, CCN concentrations were overall much lower and dominated by remote transport. These results show that anthropogenic emissions perturb CCN concentrations in remote regions that are sensitive to changes in CCN number and illustrate that accurate predictions of both transport and regional aerosol formation from the oceans are critical to accurately modeling clouds in these regions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Quantifying the effects of mixing state on aerosol optical properties

Abstract. Calculations of the aerosol direct effect on climate rely on simulated aerosol fields. The model representation of aerosol mixing state potentially introduces large uncertainties into these calculations, since the simulated aerosol optical properties are sensitive to mixing state. In this study, we systematically quantified the impact of aerosol mixing state on aerosol optical properties using an ensemble of 1800 aerosol populations from particle-resolved simulations as a basis for Mie calculations for optical properties. Assuming the aerosol to be internally mixed within prescribed size bins caused overestimations of aerosol absorptivity and underestimations of aerosol scattering. Together, these led to errors in the populations' single scattering albedo of up to −22.3 % with a median of −0.9 %. The mixing state metric χ proved useful in relating errors in the volume absorption coefficient, the volume scattering coefficient and the single scattering albedo to the degree of internally mixing of the aerosol, with larger errors being associated with more external mixtures. At the same time, a range of errors existed for any given value of χ. We attributed this range to the extent to which the internal mixture assumption distorted the particles' black carbon content and the refractive index of the particle coatings. Both can vary for populations with the same value of χ. These results are further evidence of the important yet complicated role of mixing state in calculating aerosol optical properties.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Aerosol hygroscopicity over the southeast Atlantic Ocean during the biomass burning season – Part 1: From the perspective of scattering enhancement​​​​​​​

Aerosol hygroscopicity plays a vital role in aerosol radiative forcing. One key parameter describing hygroscopicity is the scattering enhancement factor, f(RH), defined as the ratio of the scattering coefficient at humidified relative humidity (RH) to its dry value. Here, we utilize the f(80 %) from ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) 2016 and 2018 airborne measurements to investigate the hygroscopicity of aerosols, its vertical distribution, its relationship with chemical composition, and its sensitivity to organic aerosol (OA) hygroscopicity over the southeast Atlantic (SEA) Ocean during the biomass burning (BB) season. We found that aerosol hygroscopicity remains steady above 2 km, with a mean f(80 %) of 1.40 ± 0.17. Below 2 km, aerosol hygroscopicity increases with decreasing altitude, with a mean f(80 %) of 1.51 ± 0.22, consistent with higher values of BB aerosol hygroscopicity found in the literature. The hygroscopicity parameter of OA (κ OA ) is retrieved from the Mie model with a mean value of 0.11 ± 0.08, which is in the middle to upper range compared to the literature. Higher OA hygroscopicity is related to aerosols that are more aged, oxidized, and present at lower altitudes. The enhanced biomass burning aerosol (BBA) hygroscopicity at lower altitudes is mainly due to a lower OA fraction, increased sulfate fraction, and greater κ OA at lower altitudes. We propose a parameterization that quantifies f(RH) with chemical composition and κOA based on Mie simulation of internally mixed OA–(NH 4 ) 2 SO 4 –BC mixtures. The good agreement between the predictions and the ORACLES measurements implies that the aerosols in the SEA during the BB season can be largely represented by the OA–(NH 4 ) 2 SO 4 –BC internal mixture with respect to the f(RH) prediction. The sensitivity of f(RH) to κ OA indicates that applying a constant κ OA is only suitable when the OA fraction is low and κ OA shows limited variation. However, in situations deviating these two criteria, κ OA can notably impact scattering coefficients and aerosol radiative effect; therefore, accounting for κ OA variability is recommended.

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 OSTI2026

Stratospheric aerosol forcing for CMIP7 – Part 1: optical properties for pre-industrial, historical, and scenario simulations

Stratospheric aerosols, most of which originate from explosive volcanic sulfur emissions into the stratosphere, are a key natural driver of climate variability. They are thus a forcing provided by the Coupled Model Intercomparison Project (CMIP) Climate Forcings Task Team to climate modelling groups participating in phase 7 of CMIP. For the historical period, we provide two datasets covering 1750–2023: (i) a volcanic upper tropospheric-stratospheric sulfur emission dataset, documented in a companion paper; and (ii) a stratospheric sulfate aerosol optical property dataset, documented in this paper. For the satellite era (from 1979 onwards), stratospheric aerosol optical properties are derived from the Global Space-based Stratospheric Aerosol Climatology (GloSSAC) dataset. For the pre-satellite era (1750–1978), optical properties are derived from our volcanic SO 2 emission dataset using a new version of the reduced-complexity volcanic aerosol model Easy Volcanic Aerosol (Height) (EVA_H v2). A background, non-volcanic stratospheric aerosol climatology is derived from the 1998–2001 period with a trend over 1850–1978 accounting for increasing anthropogenic aerosols. A monthly stratospheric aerosol climatology is derived from the 1850–2021 average for both pre-industrial and scenario (future) simulations, with a 9-year ramp over 2022–2030 for scenario simulations to ensure a smooth transition from the historical period. CMIP7 simulations should use version 2.2.1 of our pre-industrial and historical datasets, and version 2.2.2 of our scenario dataset. Our methodology to produce historical aerosol optical properties significantly differs from CMIP6 for the pre-satellite era, and the resulting forcings in turn largely differ. In particular, the CMIP6 dataset was mostly based on the sparse and uncertain pyrheliometer record, which resulted in strongly underrepresented emissions from small-to-moderate magnitude eruptions. The resulting bias is addressed in CMIP7, which is entirely emission-derived in the pre-satellite era and uses more recent ice-core-based volcanic sulfur emission inventories than CMIP6. Our approach results in an overall larger volcanic aerosol forcing for CMIP7, with the 1850–2014 mean mid-visible global mean stratospheric aerosol optical depth (SAOD) in CMIP7 (0.0138) being 29 % higher than in CMIP6 (0.0107). The pre-industrial mean of the same variable is 26 % higher in CMIP7 (0.0135, derived from the historical 1850–2021) than CMIP6 (0.0107, derived from the historical 1850–2014 mean). Using a reduced-complexity climate model, we simulate a global mean surface temperature that is 0.07 °C colder for 1850–1900 when using the CMIP7 dataset instead of CMIP6, whereas 2000–2014 is 0.03 °C warmer in CMIP7. Our dataset also exhibits lower forcing for 1960–1980, resulting in temperatures 0.06 °C warmer when averaged over 1960–1990, a period for which CMIP6 climate models exhibit a cold bias. Given the large uncertainties characterizing the dataset, in particular for the pre-satellite era, we advise against treating the CMIP7 or CMIP6 dataset as uniquely superior for any specific year and highlight the need for further evaluation. We conclude the study by discussing sources of uncertainty for the dataset, future research avenues to improve it, as well as requirements to operationalize the production of the dataset, i.e. extend it and update it on an annual basis instead of every 5–7 years following CMIP cycles.

Aubry, Thomas J. [Univ. of Exeter, Devon (United K↗
DOE OSTI2025

Investigation of the Sensitivity of Tropical Cyclogenesis to Aerosol Intervention

Abstract As risks from tropical cyclones (TCs) are fueled by climate change escalation, there is an urgent need for transformational solutions to complement traditional approaches. Seeding TCs using aerosols can be a promising method to reduce cyclone intensity, supported by theoretical understanding of the microphysical effects of aerosols on TC clouds. The ideal time to intervene effectively in TCs is likely during their initial stage, before TC wind speeds reach their peak. However, studies exploring potential aerosol effects on TC formation remain scarce. This study investigates how a TC embryo responds to the addition of aerosols of varying sizes using the Weather Research & Forecasting (WRF) model coupled with a spectral‐bin microphysics model. We found that aerosols of different sizes and concentrations distinctively affect the pre‐TC vortex's microstructure and dynamics. Fine and ultrafine aerosols enhance the latent heat of condensation, freezing, deposition, and riming, initially intensifying the vortex. However, this results in enhancement of the cold pool, thereby reducing inflow and surface fluxes, subsequently weakening the vortex. Coarse aerosols produce the opposite effect to that of fine and ultrafine aerosols. Coarse aerosols lead to a slower initial acceleration owing to enhanced warm rain. However, the resulting weaker cold pool is insufficient to effectively reduce the strength of the vortex at the later stage. This study provides critical insights into how aerosols of varying sizes and concentrations modulate the energy cascade and impact the evolution of a TC embryo, laying the groundwork for further research on TC risk management through aerosol intervention.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Climatology Perspective of Sensitive Regimes and Active Regions of Aerosol Indirect Effect for Cirrus Clouds over the Global Oceans

Long-term satellite climate data records (CDRs) of clouds and aerosols are used to investigate the aerosol indirect effect (AIE) of cirrus clouds over the global oceans from a climatology perspective. Our study focuses on identifying the sensitive regimes and active regions where AIE signatures easily manifest themselves in the sense of the long-term average of cloud and aerosol variables. The aerosol index (AIX) regimes of AIX < 0.18 and 0.18 < AIX < 0.46 are respectively identified as the sensitive regimes for negative and positive aerosol albedos and lifetime effects of cirrus clouds. Relative humidity first decreases (along with upward motions) and then reverses to increase (along with downward motions) in the first regime of negative aerosol albedo and lifetime effects. Relatively wet and strong upward motions are the favorable meteorological conditions for the second regime of positive aerosol albedo and lifetime effects. Two swath regions extending from 15°N to 30°N over the east coastal oceans of China and the USA are the active regions of positive aerosol albedo effects. Positive aerosol lifetime effects are only active or easy to manifest in the regions where a positive aerosol albedo effect is active. The results based on the long-term averaged satellite observations are valuable for the evaluation and improvement of aerosol-cloud interactions for cirrus clouds in global climate models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Characterization of the indoor far-field aerosol transmission in a model commercial office building

As businesses gradually reopen and employees return to work, the potential spread of SARS-CoV-2 and its variants through airborne transmission via the heating, ventilation, and air-conditioning (HVAC) systems of commercial building raises concerns. Since the general practice in commercial buildings is to use low-efficiency air filters and given that indoor air is generally recycled, the degree to which cross-zone aerosol transmission occurs is of interest. To quantify the cross-zone aerosol transmission, experiments were conducted using a synthetic test aerosol in the five zones on the first floor of a model commercial office building at the Oak Ridge National Laboratory. Because the synthetic aerosol was tagged with fluorescent salt, the aerosol generated from the source zone can be distinguished from the background aerosols due to its unique fluorescent signal. Data from cross-zone campaigns showed that submicron-aerosol transmission was higher than the micron aerosols. In campaigns with doors closed, the submicron aerosol transmission was less than 16% and less than 11% for micron aerosol transmission. Finally, opening the interior doors that connecting different zones can significantly enhance the aerosol transmission for zones at the close proximity to the source, but has less impact on those farther away.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2022

Influence of Aerosol Embedded in Shallow Cumulus Cloud Fields on the Surface Solar Irradiance

Ubiquitous shallow cumulus clouds are associated with complex variability in surface solar irradiance (SSI). Aerosol embedded in the cloud field typically has a much smaller overall radiative effect, but can significantly perturb the shape of the SSI probability density function (PDF). These perturbations have important implications for several applications that utilize SSI, but are poorly quantified and are the subject of this study. Multiple cases of shallow cumulus cloud fields with embedded aerosol are simulated at the Southern Great Plains Atmospheric Observatory using large eddy simulation (LES). The LES-derived cloud and aerosol fields are then ingested into Monte Carlo three-dimensional (3D) radiative transfer to simulate SSI. We find a variety of perturbations to the SSI PDF that depend on aerosol presence and optical properties. The processes leading to these perturbations include extinction of the direct beam that often increases from the clear-sky region toward cloud edge due to aerosol hygroscopic growth, and scattering of radiation by aerosol into cloud shadows. The ability to predict the SSI PDF in the presence of aerosol is assessed by adding three representative aerosol optical properties into an existing machine learning framework. We show that machine learning accurately predicts the SSI PDF across a wide range of conditions with negligible computational expense. Importance metrics reveal the relatively high influence of aerosol optical properties in making the predictions. These new findings highlight the important role that aerosol plays in SSI variability for highly 3D cloud-aerosol environments and provides a computationally efficient route forward for its simulation.

3D radiative transfer↗