Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “AEROSOLS”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 181 records · Page 10

Improving Aerosol Radiative Forcing and Climate in E3SM: Impacts of New Cloud Microphysics and Improved Wet Removal Treatments

Abstract Numerous Earth system models exhibit excessive aerosol effective forcing at the top of the atmosphere (TOA), including the Department of Energy's Energy Exascale Earth System Model (E3SM). Here, in the context of the E3SM version 3 effort, the predicted particle property (P3) stratiform cloud microphysics scheme and an enhanced deep convection parameterization suite (ZM_plus) are implemented into E3SM. The ZM_plus includes a convective cloud microphysics scheme, a multi‐scale coherent structure parameterization for mesoscale convective systems, and a revised cloud base mass flux formulation considering impacts of the large‐scale environment. The P3 scheme improved cloud and radiation particularly over the Northern Hemisphere and the frequency of heavy precipitation over the tropics, and the ZM_plus improved clouds in the tropics. P3 decreases aerosol effective forcing by 0.15 W m −2 , while the ZM_plus increases it by 0.27 W m −2 , resulting from excessive direct (0.31 W m −2 ) and indirect forcing (−1.79 W m −2 ). The excessive aerosol forcings are due to aerosol overestimation associated with insufficient aerosol wet removal. By improving the physical treatments in the aerosol wet removal, we effectively mitigate anthropogenic aerosol overestimation and thus attenuate direct (0.09 W m −2 ) and indirect aerosol forcing (−1.52 W m −2 ). Adjustment to primary organic matter hygroscopicity reduces direct and indirect forcing to more reasonable values: −0.13 W m −2 and −1.31 W m −2 , respectively. On climatology, improved aerosol treatments mitigate overestimation of aerosol optical depth.

54 ENVIRONMENTAL SCIENCES↗

Influence of biogenic emissions from boreal forests on aerosol–cloud interactions

Boreal forest acts as a carbon sink and contributes to the formation of secondary organic aerosols via emission of aerosol precursor compounds. However, these influences on the climate system are poorly quantified. Here we show direct observational evidence that aerosol emissions from the boreal forest biosphere influence warm cloud microphysics and cloud-aerosol interactions in a scale-dependent and highly dynamic manner. Analyses of in situ and ground-based remote-sensing observations from the SMEAR II station in Finland, conducted over eight months in 2014, reveal substantial increases in aerosol load over the forest one to three days after aerosol-poor marine air enters the forest environment. We find that these changes are consistent with secondary organic aerosol formation and, together with water-vapour emissions from evapotranspiration, are associated with changes in the radiative properties of warm, low-level clouds. Here, the feedbacks between boreal forest emissions and aerosol-cloud interactions and the highly dynamic nature of these interactions in air transported over the forest over timescales of several days suggest boreal forests have the potential to mitigate climate change on a continental scale. Our findings suggest that even small changes in aerosol precursor emissions, whether due to changing climatic or anthropogenic factors, may substantially modify the radiative properties of clouds in moderately polluted environments. Emissions from the boreal forest biosphere can substantially increase aerosol load above the forest and influence the radiative properties of clouds, according to analysis of observations from a monitoring station in Finland.

54 ENVIRONMENTAL SCIENCES↗

Aerosol-boundary layer interaction modulated entrainment process

Abstract Aerosol-boundary layer interactions play an important role in affecting atmospheric thermodynamics and air pollution. As a key factor in dictating the development of the boundary layer, the entrainment process in the context of aerosol-boundary layer interactions is still poorly understood. Using comprehensive field observations made at a superstation in Beijing, we gain insight into the response of the entrainment process to aerosols. We found that high aerosol loading can significantly suppress the entrainment rate, breaking the conventional linear relationship between sensible heat fluxes and entrainment fluxes. Related to aerosol vertical distributions, aerosol heating effects can alter vertical heat fluxes, leading to a strong interaction between aerosols and the entrainment process in the upper boundary layer. Such aerosol-entrainment coupling can inhibit boundary layer development and explains the great sensitivity of observed entrainment rates to aerosols than can traditional calculations. The notable impact of aerosols on the entrainment process raises holistic thinking about the dynamic framework of the boundary layer in a polluted atmosphere, which may have a significant bearing on the dispersion of air pollutants and the land-atmosphere coupling.

54 ENVIRONMENTAL SCIENCES↗

Understanding aerosol properties in convective outflows during TRACER

Convective outflow boundaries commonly form across the southeastern U.S., often originating from storms initiated along sea-breeze fronts. As outflows spread, merge, and collide, they frequently trigger secondary convection in air masses already modified by primary storm outflow. This resulting air mass carries a distinctive aerosol population, which can influence the development of secondary convective cells. During the U.S. DOE TRACER field campaign in summer 2022, we investigated how outflows affect aerosol size, composition, and hygroscopicity across Greater Houston, Texas. Using a novel detection algorithm, we identified and verified 72 outflow boundaries from surface meteorological observations. In the relatively simple continental environment northwest of Houston, a common relationship emerged between CCN-inferred hygroscopicity (κ) and size-resolved aerosol concentrations. The κ of aerosols typically decreased in size ranges where aerosol concentrations increased following outflow passage and increased where concentrations decreased. In contrast, at the Atmospheric Radiation Measurement’s (ARM) fixed site in La Porte, Texas, the aerosol response depended on outflow direction, shaped by concentrated industrial and shipping activity to the north and south/southeast along the Houston Ship Channel. Concurrent size distribution and composition changes suggested case-specific variability in κ, with either reinforcing or offsetting effects. Outflows passing over industrial/shipping sectors often promoted less hygroscopic aerosol populations while cleaner residential outflows often favored more hygroscopic aerosol populations. These results highlight key aerosol changes following outflow passage, providing a foundation for improved understanding of aerosol-cloud interactions related to secondary convection initiation along or in the wake of outflow boundaries.

Thompson, Seth A. [Texas A & M Univ., College Stat↗

Isolating the effect of biomass burning aerosol emissions on 20th century hydroclimate in South America and Southeast Asia

Abstract Biomass burning is a significant source of aerosol emissions in some regions and has a considerable impact on regional climate. Earth system model simulations indicate that increased biomass burning aerosol emissions contributed to statistically significant decreases in tropical precipitation over the 20th century. In this study, we use the Community Earth System Model version 1 Large Ensemble (CESM1-LENS) experiment to evaluate the mechanisms by which biomass burning aerosol contributed to decreased tropical precipitation, with a focus on South America and Southeast Asia. We analyze the all-but-one forcing simulations in which biomass burning aerosol emissions are held constant while other forcings (e.g., greenhouse gas concentrations) vary throughout the 20th century. This allows us to isolate the influence of biomass burning aerosol on processes that contribute to decreasing precipitation, including cloud microphysics, the radiative effects of absorbing aerosol particles, and alterations in regional circulation. We also show that the 20th century reduction in precipitation identified in the CESM1-LENS historical and biomass burning experiments is consistent across Coupled Model Intercomparison Project Phase 5 models with interactive aerosol schemes and the CESM2 single-forcing experiment. Our results demonstrate that higher concentrations of biomass burning aerosol increases the quantity of cloud condensation nuclei and cloud droplets, limiting cloud droplet size and precipitation formation. Additionally, absorbing aerosols (e.g., black carbon) contribute to a warmer cloud layer, which promotes cloud evaporation, increases atmospheric stability, and alters regional circulation patterns. Corresponding convectively coupled circulation responses, particularly over the tropical Andes, contribute to further reducing the flow of moisture and moisture convergence over tropical land. These results elucidate the processes that affect the water cycle in regions prone to biomass burning and inform our understanding of how future changes in aerosol emissions may impact tropical precipitation over the 21st century.

Environmental Sciences & Ecology↗

Arctic Aerosol Sources and Mixing States Field Campaign Report

The Arctic is warming at a faster rate than anywhere else on Earth, with rapidly shrinking sea ice extent transforming the region. Depending on chemical and physical properties, atmospheric aerosols directly scatter and/or absorb radiation, serve as cloud droplet and/or ice crystal nuclei, and/or reduce the reflectiveness of the snow surface, thereby altering the atmospheric energy budget. There is a wide spread in the magnitude of simulated arctic aerosol radiative forcing, and significant differences in aerosol concentration levels and seasonal cycles often exist between models and observations. Increasing local natural and anthropogenic emissions are significant, with uncertain climate impacts due to complex feedbacks. Model evaluations, however, are limited by the dearth of arctic aerosol observations available and an inadequate understanding of arctic aerosol processes. The majority of previous arctic aerosol observations have been made through intensive spring/summer field campaigns, with few intensive measurement studies focused on the fall-winter transition, a period when freeze-up is occurring later and thinning sea ice is resulting in wintertime ice fracturing. Aerosol monitoring at arctic coastal stations has provided knowledge of long-term seasonal trends in aerosol concentrations. The completed ARM field campaign addresses observational and knowledge gaps through detailed aerosol size and chemical composition measurements during the fall-winter transition in the coastal Arctic and through the entire annual cycle in the central Arctic. The observations are improving our understanding of the sources and processes controlling the aerosol population in the rapidly changing Arctic.

54 ENVIRONMENTAL SCIENCES↗

Tracking Aerosol Convection Interactions Experiment (TRACER) Field Campaign Report

Convective clouds serve a critical role in the Earth’s energy and water cycles through their transport of heat, moisture, momentum, and chemical species through the troposphere driving the global circulation (e.g., Hartmann et al. 1984, Del Genio et al. 2012, Su et al. 2014). On more local scales, convective clouds impact the atmospheric heating profile through diabatic heating effects, removal of water from the atmospheric column through precipitation, and conditioning of the local environment impacting further development of clouds (e.g., Sullivan and Voigt 2021). These critical roles underscore the importance of realistic representation of convective processes across scales of models from large-eddy simulation (LES), to convection-permitting models (CPM; e.g., Kendon et al. 2020, Marinescu et al. 2021), to numerical weather prediction (NWP) models used for operational weather forecasting, to Earth system models used to predict climate sensitivity (Sanderson et al. 2011, Sherwood et al. 2014, Tomassini et al. 2014, Zhao et al. 2016, Cronin et al. 2017). A key component of improving model representation of convective clouds is better quantification and parameterization of updraft microphysics and dynamics, including their interactions with the surrounding environment and storm organization (Bony et al. 2015, Hagos and Houze 2016, Donner et al. 2016, Morrison et al. 2020). Aerosol is an important environmental factor that could affect convective clouds and precipitation since cloud droplet and ice formation processes are initiated by it. Andrae et al. (2004) hypothesized that aerosols associated with increased biomass burning particles acting as cloud condensation nuclei (CCN) result in smaller and more monodisperse cloud droplets leading to suppression of warm rain formation, ultimately leading to more cloud water being lofted above the freezing level based on observations in the Amazon region. The subsequent increase in latent heat release increases the buoyancy of rising convective parcels invigorating the deep convection. This work was followed by a description of the theoretical basis for this “cold-phase invigoration” by Rosenfeld et al. (2008), who argued that it could have a significant effect for deep convective clouds with warm cloud-bases. Several modeling studies (e.g., Khain et al. 2005, 2009, van den Heever et al. 2006, Fan et al. 2007, 2009, 2012, Lee et al. 2008, Storer et al. 2010, Lebo et al. 2012, Storer and van den Heever 2013, Chen et al. 2020, Dagan et al. 2022) have investigated these aerosol-convection interactions and the environmental factors that influence their relative importance and magnitude. More recently, several studies have indicated that “warm-phase invigoration”, the enhancement of convection through condensational heating, also appears to play a role in enhancing both shallow cumuli (Seiki and Nakajima 2014, Saleeby et al 2015) and deeper tropical convection (Lebo and Seinfeld 2011, Khain et al. 2012, Sheffield et al 2015, Fan et al. 2018, Igel and van den Heever 2021), as well as Houston thunderstorms (Fan et al. 2007, 2020). However, still other studies have provided additional evidence of systematic biases in simulated convective outflow ice size distribution properties, which are consistent with a lack of poorly understood secondary ice production within convective updrafts (e.g., Fridlind et al. 2017). To help address these critical gaps in our understanding of cloud processes, aerosol processes and aerosol-cloud interactions, the Tracking Aerosol Convection Interactions Experiment was designed building upon efforts by the Aerosol, Cloud, Precipitation and Climate (ACPC) Initiative (http://acpcintiative.org/), a joint effort of the International Geosphere-Biosphere Programme (IGBP) and the World Climate Research Program (WCRP) that focused on resolving uncertainties in the interactions between aerosol and clouds towards better understanding the role that these interactions play in the climate system. The TRACER campaign was motivated by recommendations from a number of pilot studies undertaken by ACPC (van den Heever et al. 2017, Fridlind et al. 2019, Hu et al. 2019, Fan et al. 2020, Marinescu et al. 2021, Hernandez-Deckers et al. 2022) that pointed towards the southeastern Texas region as a locale where aerosol-convection interactions could be studied owing to the copious occurrence of isolated convection during the summer months accompanied by diverse and significant sources of aerosols from both anthropogenic and natural sources. The TRACER campaign began on 01 October 2021 and extended through 30 September 2022 with an intensive operational period (IOP) during June-September 2022. Three main sites (Table 1) were managed by the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility.

54 ENVIRONMENTAL SCIENCES↗

Cloud Processing of Aerosol during SAIL Field Campaign Report

Globally, on average, the release rate of aerosols from clouds is estimated to be about 6,000 Tg/yr and an aerosol particle is estimated to experience about three cloud cycles. Cloud processing of aerosol produces aerosols that have dramatically different physicochemical properties compared to their original form. Cloud processing may transform particles to efficient cloud condensation nuclei (CCN) or ice nucleating particles (INP) that can further participate in cloud formation. We investigated cloud processing of aerosol during the U.S. Department of Energy (DOE)’s Atmospheric Radiation Measurement (ARM) Surface Atmosphere Integrated Field Laboratory (SAIL) field campaign using multi-modal offline analysis techniques available at DOE’s Environmental Molecular Sciences Laboratory (EMSL). The main scientific aim of this project was to understand the processes that transform aerosols (chemically, and physically), and influence aerosol-cloud interactions. Aerosol particles undergo significant modifications due to warm (cloud droplets) and cold cloud (ice crystals) processing. Cloud processing of aerosol has important effects on the atmospheric aerosol number and mass concentration, size distribution, phase separation, and chemical composition.

54 ENVIRONMENTAL SCIENCES↗

FY23 Update: Aerosol Sampling for the Canister Deposition Field Demonstration

This report describes the results of preliminary testing of aerosol monitoring equipment that will be used to continuously monitor the aerosol source term for the multi-year Canister Deposition Field Demonstration (CDFD). These data are required inputs for the development and validation of models for the deposition of dust and potentially corrosive salts on the surface of spent nuclear fuel (SNF) dry storage canisters. Surface salt loads correlate with the extent of corrosion damage on a metal surface, and potentially to the likelihood and timing of initiation of stress corrosion cracks. Aerosols will be monitored at the CDFD site using three instruments. A Dekati ® ELPI+ cascade impactor will be used for real-time monitoring of aerosol particle sizes. It will also collect dust in 14 size bins on impactor targets that can be chemically analyzed to determine the soluble salts present as a function of particle size. However, this instrument can only measure dried aerosols, with a diameter of <10 µm. The second instrument is a Topas laser particle size spectrometer, which provides real-time monitoring of aerosol particle sizes up to ~40 µm in size. It monitors both the ambient (potentially deliquesced) aerosol particle size distributions required for the dust deposition models and the distributions of the equivalent dried particles, allowing correlation with the Dekati ® data. However, it does not discriminate between inert dust particles and salt aerosols, and it does not retain samples of the different particle sizes for later analysis. The third instrument that will monitor aerosols at the CDFD site is a Clean Air Status and Trends Network (CASTNET) tower, which uses a multiple canister system to collect weekly samples for analysis to total suspended aerosol particle compositions and atmospheric gas concentrations. This status report describes work in FY23 to develop the capabilities for using these tools. In two training exercises, the cascade impactor and laser particle sizer were deployed in two different testing environments, one indoor and one outdoor. For the cascade impactor, the tests provided opportunities for the operators to familiarize themselves with impactor substrate preparation, and post-test sample removal and analysis. For the laser particle sizer, the tests were used to evaluate different instrument parameters, to determine the most appropriate settings for capturing transient events. Data and samples were collected for weeks to months for each test, and the results are presented here. In addition to the preliminary testing, contracts were developed with WSP Analytical Labs for sample preparation and analysis of the cascade impactor samples. The impactor tower from outdoor test was delivered to WSP and used to train the staff there in disassembly, sample extraction, sample analysis, and tower reassembly with new target substrates. These are tasks that WSP will be performing routinely for the CDFD project. The CASTNET system cannot be purchased or tested until an actual site has been selected for the CDFD test. Work for this FY has been restricted to preparation of contracts for purchasing the CASTNET tower, and for sample analysis, once the tower is in operation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Method for Real-Time Salt Aerosol Concentration and Size Measurements for Molten Salt Reactor Safety Assessments

Licensing a new nuclear reactor involves evaluating credible accident scenarios by developing models that simulate accident progression to predict possible outcomes and their impact on safety. The formation of radionuclide-bearing aerosols in the respirable size range can significantly affect dose consequence and threaten human health and is therefore a focus of nuclear reactor safety assessments. Recent reviews of the literature identified a lack of existing experimental data describing the mechanisms of formation and properties (size, concentration, and composition) of radionuclide-bearing aerosols that may be produced from molten salt reactor (MSR) facilities during postulated accident scenarios. Experiments on aerosol formation from molten salt systems are a high priority need that will support MSR licensing by indicating the radiological consequences of aerosol formation and providing the data required for model development and validation. The evolving conditions that occur during a MSR accident, such as a spill of molten fuel salt, may affect aerosol formation mechanisms and aerosol properties over time. There is a need to conduct experiments that simulate credible MSR accidents in a laboratory to generate aerosols with realistic characteristics and behaviors and a need to measure these aerosols in real time under accident-relevant conditions. This report describes the development of a method that can be used to quantify the size and concentration of salt aerosol particles that form from molten salt systems in real time. This method 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 that will provide mechanistic insight into aerosol formation and properties to support process model development.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Understanding Aitken Mode Aerosol Variability over the Southern Ocean and Antarctica: Insights from Cloud Condensation Nuclei Data

Aitken mode aerosol particles play an important role influencing cloud properties and sustenance, acting as a reservoir of potential cloud condensation nuclei against precipitation scavenging. However, there is limited data on Aitken mode aerosols. In this study, we develop a method to estimate Aitken mode aerosol concentrations and size distribution using cloud condensation nuclei measurements (CCN) and κ-Köhler theory. The performance of this method is evaluated using scanning mobility particle sizer (SMPS) data from recent field campaigns to demonstrate its skills and applicability. The method reasonably estimates Aitken- and accumulation-mode aerosol concentrations, achieving correlations of 0.7–0.9 with only modest biases (mean fractional bias within ±23% for Aitken mode and ±34% for accumulation-mode). This method is further applied to measurements collected over the Southern Ocean and Antarctica in recent years from multiple platforms, including ground sites, aircraft, and ships, to derive Aitken and accumulation-mode aerosol concentrations. Using the derived data, we examine the seasonal cycle, latitudinal variations, and vertical distribution of aerosols. Aitken mode aerosol concentrations are elevated over the Southern Ocean and Antarctica during the austral summer similar to the accumulation mode. In the austral summer, the free troposphere has more Aitken mode aerosols and fewer accumulation mode aerosols than the boundary layer, and thus likely serves as an important source of cloud-forming aerosol while also diluting the accumulation mode.

Kang, Litai [University of Washington] (ORCID:0000↗

Seasonal Variation of Dust Aerosol Vertical Distribution in Arctic Based on Polarized Micropulse Lidar Measurement

This study investigates the seasonal variation of dust aerosol vertical distribution using polarized Micropulse lidar (MPL) measurements at the Atmospheric Radiation Measurement (ARM) North Slope of Alaska (NSA) observatory from January 2013 to September 2017. For the first time, multi-year aerosol backscatter coefficients are retrieved at the ARM NSA site from MPL measurements and are consistent with co-located high spectral resolution lidar (HSRL) measurements. The high-quality aerosol backscatter coefficient retrievals are used to derive the particle depolarization ratio (PDR) at the wavelength of 532 nm, which is used to identify the presence of dust aerosols. The annual cycles of the vertical distributions of dust backscatter coefficient and PDR and dust aerosol optical depth (DAOD) show that aerosol loading has a maximum in late winter and early spring but a minimum in late summer and early autumn. Vertically, dust aerosol occurs in the entire troposphere in spring and winter and in the low and middle troposphere in summer and autumn. Because dust aerosols are effective ice nuclei, the seasonality of dust aerosol vertical distribution has important implications for the Arctic climate through aerosol–cloud–radiation interactions, primarily through impacting mixed-phase cloud processes.

47 OTHER INSTRUMENTATION↗

Cloud drop number concentrations over the western North Atlantic Ocean: seasonal cycle, aerosol interrelationships, and other influential factors

Cloud drop number concentrations (N d ) over the western North Atlantic Ocean (WNAO) are generally highest during the winter (DJF) and lowest in summer (JJA), in contrast to aerosol proxy variables (aerosoloptical depth, aerosol index, surface aerosol mass concentrations, surface cloud condensation nuclei (CCN) concentrations) that generally peak inspring (MAM) and JJA with minima in DJF. Using aircraft, satellite remote sensing, ground-based in situ measurement data, and reanalysis data, we characterize factors explaining the divergent seasonal cycles and furthermore probe into factors influencing N d on seasonal timescales. The results can be summarized well by features most pronounced in DJF, including features associated with cold-air outbreak (CAO) conditions such as enhanced values of CAO index, planetary boundary layer height (PBLH),low-level liquid cloud fraction, and cloud-top height, in addition to winds aligned with continental outflow. Data sorted into high- and low-N d days in each season, especially in DJF, revealed that all of these conditions were enhanced on the high-N d days, including reduced sea level pressure and stronger wind speeds. Although aerosols may be more abundant in MAM and JJA, the conditions needed to activate those particles into cloud droplets are weaker than in colder months, which is demonstrated by calculations of the strongest (weakest) aerosol indirect effects in DJF (JJA) based on comparing N d to perturbations in four different aerosol proxy variables (total and sulfate aerosol optical depth, aerosol index, surface mass concentration of sulfate). We used three machine learning models and up to 14 input variables to infer about most influential factors related to N d for DJF and JJA, with the best performance obtained with gradient-boosted regression tree (GBRT) analysis. The model results indicated that cloud fraction was the most important input variable, followed by some combination (depending on season) of CAO index and surface mass concentrations of sulfate and organic carbon. Future work is recommended to further understand aspects uncovered here such as impacts of free tropospheric aerosol entrainment on clouds, degree of boundary layer coupling, wet scavenging, and giant CCN effects on aerosol–N d relationships, updraft velocity, and vertical structure of cloud properties such as adiabaticity that impact the satellite estimation of N d .

54 ENVIRONMENTAL SCIENCES↗

Atmospheric particle abundance and sea salt aerosol observations in the springtime Arctic: a focus on blowing snow and leads

Abstract. Sea salt aerosols play an important role in the radiation budget and atmospheric composition over the Arctic, where the climate is rapidly changing. Previous observational studies have shown that Arctic sea ice leads are an important source of sea salt aerosols, and modeling efforts have also proposed blowing snow sublimation as a source. In this study, size-resolved atmospheric particle number concentrations and chemical composition were measured at the Arctic coastal tundra site of Utqiaġvik, Alaska, during spring (3 April–7 May 2016). Blowing snow conditions were observed during 25 % of the 5-week study period and were overpredicted by a commonly used blowing snow parameterization based solely on wind speed and temperature. Throughout the study, open leads were present locally. During periods when blowing snow was observed, significant increases in the number concentrations of 0.01–0.06 µm particles (factor of 6, on average) and 0.06–0.3 µm particles (67 %, on average) and a significant decrease (82 %, on average) in 1–4 µm particles were observed compared to low wind speed periods. These size distribution changes were likely caused by the generation of ultrafine particles from leads and/or blowing snow, with scavenging of supermicron particles by blowing snow. At elevated wind speeds, both submicron and supermicron sodium and chloride mass concentrations were enhanced, consistent with wind-dependent local sea salt aerosol production. At moderate wind speeds below the threshold for blowing snow as well as during observed blowing snow, individual sea spray aerosol particles were measured. These individual salt particles were enriched in calcium relative to sodium in seawater due to the binding of this divalent cation with organic matter in the sea surface microlayer and subsequent enrichment during seawater bubble bursting. The chemical composition of the surface snowpack also showed contributions from sea spray aerosol deposition. Overall, these results show the contribution of sea spray aerosol production from leads on both aerosols and the surface snowpack. Therefore, if blowing snow sublimation contributed to the observed sea salt aerosol, the snow being sublimated would have been impacted by sea spray aerosol deposition rather than upward brine migration through the snowpack. Sea spray aerosol production from leads is expected to increase, with thinning and fracturing of sea ice in the rapidly warming Arctic.

54 ENVIRONMENTAL SCIENCES↗

Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing

Abstract. Aerosol indirect radiative forcing (IRF), which characterizes how aerosols alter cloud formation and properties, is very sensitive to the preindustrial (PI) aerosol burden. Dimethyl sulfide (DMS), emitted from the ocean, is a dominant natural precursor of non-sea-salt sulfate in the PI and pristine present-day (PD) atmospheres. Here we revisit the atmospheric oxidation chemistry of DMS, particularly under pristine conditions, and its impact on aerosol IRF. Based on previous laboratory studies, we expand the simplified DMS oxidation scheme used in the Community Atmospheric Model version 6 with chemistry (CAM6-chem) to capture the OH-addition pathway and the H-abstraction pathway and the associated isomerization branch. These additional oxidation channels of DMS produce several stable intermediate compounds, e.g., methanesulfonic acid (MSA) and hydroperoxymethyl thioformate (HPMTF), delay the formation of sulfate, and, hence, alter the spatial distribution of sulfate aerosol and radiative impacts. The expanded scheme improves the agreement between modeled and observed concentrations of DMS, MSA, HPMTF, and sulfate over most marine regions, based on the NASA Atmospheric Tomography (ATom), the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA), and the Variability of the American Monsoon Systems (VAMOS) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) measurements. We find that the global HPMTF burden and the burden of sulfate produced from DMS oxidation are relatively insensitive to the assumed isomerization rate, but the burden of HPMTF is very sensitive to a potential additional cloud loss. We find that global sulfate burden under PI and PD emissions increase to 412 Gg S (+29 %) and 582 Gg S (+8.8 %), respectively, compared to the standard simplified DMS oxidation scheme. The resulting annual mean global PD direct radiative effect of DMS-derived sulfate alone is −0.11 W m−2. The enhanced PI sulfate produced via the gas-phase chemistry updates alone dampens the aerosol IRF as anticipated (−2.2 W m−2 in standard versus −1.7 W m−2, with updated gas-phase chemistry). However, high clouds in the tropics and low clouds in the Southern Ocean appear particularly sensitive to the additional aqueous-phase pathways, counteracting this change (−2.3 W m−2). This study confirms the sensitivity of aerosol IRF to the PI aerosol loading and the need to better understand the processes controlling aerosol formation in the PI atmosphere and the cloud response to these changes.

54 ENVIRONMENTAL SCIENCES↗

Opinion: A critical evaluation of the evidence for aerosol invigoration of deep convection

Deep convective updraft invigoration via indirect effects of increased aerosol number concentration on cloud microphysics is frequently cited as a driver of correlations between aerosol and deep convection properties. Here, we critically evaluate the theoretical, modeling, and observational evidence for warm- and cold-phase invigoration pathways. Though warm-phase invigoration is plausible and theoretically supported via lowering of the supersaturation with increased cloud droplet concentration in polluted conditions, the significance of this effect depends on substantial supersaturation changes in real-world convective clouds that have not been observed. Much of the theoretical support for cold-phase invigoration depends on unrealistic assumptions of instantaneous freezing and unloading of condensate in growing, isolated updrafts. When applying more realistic assumptions, impacts on buoyancy from enhanced latent heating via fusion in polluted conditions are largely canceled by greater condensate loading. Many foundational observational studies supporting invigoration have several fundamental methodological flaws that render their findings incorrect or highly questionable. Thus, much of the evidence for invigoration has come from numerical modeling, but different models and setups have produced a vast range of results. Furthermore, modeled aerosol impacts on deep convection are rarely tested for robustness, and microphysical biases relative to observations persist, rendering many results unreliable for application to the real world. Without clear theoretical, modeling, or observational support, and given that enervation rather than invigoration may occur for some deep convective regimes and environments, it is entirely possible that the overall impact of cold-phase invigoration is negligible. Substantial mesoscale variability of dominant thermodynamic controls on convective updraft strength coupled with substantial updraft and aerosol variability in any given event are poorly quantified by observations and present further challenges to isolating aerosol effects. Observational isolation and quantification of convective invigoration by aerosols is also complicated by limitations of available cloud condensation nuclei and updraft speed proxies, aerosol correlations with meteorological conditions, and cloud impacts on aerosols. Furthermore, many cloud processes, such as entrainment and condensate fallout, modulate updraft strength and aerosol–cloud interactions, varying with cloud life cycle and organization, but these processes remain poorly characterized. Considering these challenges, recommendations for future observational and modeling research related to aerosol invigoration of deep convection are provided.

54 ENVIRONMENTAL SCIENCES↗

Chemical properties and single-particle mixing state of soot aerosol in Houston during the TRACER campaign

Abstract. A high-resolution soot particle aerosol mass spectrometer (SP-AMS) was used to selectively measure refractory black carbon (rBC) and its associated coating material using both the ensemble size-resolved mass spectral mode and the event trigger single particle (ETSP) mode in Houston, Texas, in summer 2022. This study was conducted as part of the Department of Energy Atmospheric Radiation Measurement (ARM) program's TRacking Aerosol Convection interactions ExpeRiment (TRACER) field campaign. The study revealed an average (±1σ) rBC concentration of 103 ± 176 ng m−3. Additionally, the coatings on the BC particles were primarily composed of organics (59 %; 219 ± 260 ng m−3) and sulfate (26 %; 94 ± 55 ng m−3). Positive matrix factorization (PMF) analysis of the ensemble mass spectra of BC-containing particles resolved four distinct types of soot aerosol, including an oxidized organic aerosol (OOABC,PMF) factor associated with processed primary organic aerosol, an inorganic sulfate factor (SO4,BC,PMF), an oxidized rBC factor (O-BCPMF), and a mixed mineral dust–biomass burning aerosol factor with significant contribution from potassium (K-BBBC,PMF). Additionally, K-means clustering analysis of the single-particle mass spectra identified eight different clusters, including soot particles enriched in hydrocarbon-like organic aerosol (HOABC,ETSP), sulfate (SO4,BC,ETSP), two types of rBC, OOA (OOABC,ETSP), chloride (ClBC,ETSP), and nitrate (NO3,BC,ETSP). The single-particle measurements demonstrate substantial variation in BC coating thickness with coating-to-rBC mass ratios ranging from 0.1 to 100. The mixing state index (χ), which denotes the degree of homogeneity of the soot aerosol, varied from 4 % to 94 % with a median of 40 %, indicating that the aerosol population lies in between internal and external mixing but has large temporal and source type variability. In addition, a significant fraction of BC-containing particles, a majority enriched with oxidized organics and sulfate, exhibit sufficiently high κ values and diameters conducive to activation as cloud nuclei under atmospherically relevant supersaturation conditions. This finding bears significance in comprehending the aging processes of rBC-containing particles and their activation into cloud droplets. Our analysis highlights the complex nature of soot aerosol and underscores the need to comprehend its variability across different environments for accurate assessment of climate change.

54 ENVIRONMENTAL SCIENCES↗

High sensitivity of simulated fog properties to parameterized aerosol activation in case studies from ParisFog

Aerosols influence fog properties such as visibility and lifetime by affecting fog droplet number concentrations (N d ). Numerical weather prediction (NWP) models often represent aerosol–fog interactions using highly simplified approaches. Incorporating prognostic size-resolved aerosol microphysics from climate models could allow them to simulate N d and aerosol–fog interactions without incurring excessive computational expense. However, microphysics code designed for coarse spatial resolution may struggle with sub-kilometer-scale grid spacings. Here, we test the ability of the UK Met Office Unified Model to simulate aerosol and fog properties during case studies from the ParisFog field campaign in 2011. We examine the sensitivity of fog properties to variations in N d caused by modifications to simulated aerosol activation. Our model, with a 500 m horizontal resolution and interactive aerosol and cloud microphysics, significantly underpredicts N d , although it only slightly underestimates the cloud condensation nuclei concentration. With an updated version of the Abdul-Razzak and Ghan (2000) activation scheme, we produce N d that are more consistent with those predicted by a cloud parcel model under fog-like conditions. We activate droplets only by adiabatic cooling. We incorporate more realistic hygroscopicities for sulfate and organic aerosols and explore the sensitivity of simulated N d to unresolved updrafts. We find that both N d and simulated fog liquid water content are very sensitive to the updated activation scheme but remain less affected by the update to hygroscopicities. Our improvements offer insights into the physical processes regulating N d in stable conditions, potentially laying foundations for improved operational fog forecasts that incorporate interactive aerosol simulations or aerosol climatologies.

Ghosh, Pratapaditya [Carnegie Mellon University, P↗