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DOE OSTI2026

Corrected Moments in Antenna Coordinates (CMAC) Technical Report

Various corrections are needed in order to extract the best value of the measurements from the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) User Facility’s scanning precipitation radars. The Corrected Moments in Antenna Coordinates (CMAC) Value-Added Product provides an application chain for providing radar moments that are corrected for artifacts such as aliasing, attenuation, multi-trip echoes, and beam blockage. This technical report provides details on the entire process of correcting the ARM scanning precipitation radar data using CMAC. CMAC has been used at multiple ARM sites and ARM Mobile Facility deployments including the Tracking Aerosol Convection Interactions Experiment (TRACER), Cloud, Aerosol, and Complex Terrain Interactions (CACTI), and the Surface Atmosphere Integrated Laboratory (SAIL).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Size-resolved Eddy-Covariance Particle Flux Measurement during the TRACER Campaign (Final Report)

The main goal of the TRacking Aerosol Convection interactions ExpeRiment (TRACER) campaign was to study aerosol–cloud interactions during deep convection over the Houston area. This project deployed a suite of instrumentation with the aim to (1) quantify turbulent vertical particle fluxes during at DOE-ARM sites, including TRACER, (2) assess hygroscopic growth factors and hygroscopicity parameters of the material driving modal aerosol growth during new particle formation and growth events, (3) derive turbulent aerosol mass fluxes using co-located Doppler LIDAR measurements, and (4) create quality-controlled PI data products to support future research utilizing data collected during the TRACER campaign. This report summarized the main findings from the deployments at two DOE-ARM sites. Briefly, we found that new particle formation may occur aloft, in a residual layer, near the top of the boundary layer. Small grown particles appear later due to downward mixing with daytime turbulence. The species that are responsible for aerosol modal growth had hygroscopicity parameters varying between 0.05 and 0.34. These values systematically depended on the wind sector, suggesting that the chemical composition of the precursors differed. This work demonstrated that lidar retrievals of the elastic backscatter and Doppler velocity can be used to obtain surface number emissions of particles with a diameter greater than 0.53 µm. During TRACER, emission particle number fluxes peaked near ∼ 100 cm−2 s−1. Multiple quality-controlled PI data products that will support future TRACER related science were generated and made publically available.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Source attribution of Arctic black carbon and sulfate aerosols and associated Arctic surface warming during 1980–2018

Observations show that the concentrations of Arctic sulfate and black carbon (BC) aerosols have declined since the early 1980s. Previous studies have reported that reducing sulfate aerosols potentially contributed to the recent rapid Arctic warming. In this study, a global aerosol–climate model (Community Atmosphere Model, version 5) equipped with Explicit Aerosol Source Tagging (CAM5-EAST) is applied to quantify the source apportionment of aerosols in the Arctic from 16 source regions and the role of aerosol variations in affecting changes in the Arctic surface temperature from 1980 to 2018. The CAM5-EAST simulated surface concentrations of sulfate and BC in the Arctic had a decrease of 43% and 23%, respectively, in 2014–2018 relative to 1980–1984 mainly due to the reduction of emissions from Europe, Russia and local Arctic sources. Increases in emissions from South and East Asia led to positive trends in Arctic sulfate and BC in the upper troposphere. All aerosol radiative impacts are considered including aerosol–radiation and aerosol–cloud interactions, as well as black carbon deposition on snow- and ice-covered surfaces. Within the Arctic, sulfate reductions caused a top-of-atmosphere (TOA) warming of 0.11 and 0.25 W m -2 through aerosol–radiation and aerosol–cloud interactions, respectively. While the changes in Arctic atmospheric BC has little impact on local radiative forcing, the decrease in BC in snow and ice led to a net cooling of 0.05 W m -2 . By applying climate sensitivity factors for different latitudinal bands, global changes in sulfate and BC during 2014–2018 (with respect to 1980–1984) exerted a +0.088 and 0.057 K Arctic surface warming, respectively, through aerosol–radiation interactions. Through aerosol–cloud interactions, the sulfate reduction caused an Arctic warming of +0.193 K between the two time periods. The weakened BC effect on snow–ice albedo led to an Arctic surface cooling of -0.041 K. The changes in atmospheric sulfate and BC outside the Arctic produced a total Arctic warming of +0.25 K, the majority of which is due to the midlatitude changes in radiative forcing. Our results suggest that changes in aerosols over the midlatitudes of the Northern Hemisphere have a larger impact on Arctic temperature than other regions through enhanced poleward heat transport. The combined total effects of sulfate and BC produced an Arctic surface warming of +0.297 K, explaining approximately 20% of the observed Arctic warming since the early 1980s.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Reconciling Contrasting Relationships Between Relative Dispersion and Volume-Mean Radius of Cloud Droplet Size Distributions

Cloud droplet spectral relative dispersion is critical to parameterizations of cloud radiative properties, warm-rain initiation, and aerosol-cloud interactions in models; however, there is no consistent relationship between relative dispersion and volume-mean radius in literature, which hinders improving relative dispersion parameterization and calls for physical explanation. Here we show, by analyzing aircraft observations of cumulus clouds during Routine AAF [Atmospheric Radiation Measurement (ARM) Aerial Facility] Clouds with Low Optical Water Depths (CLOWD) Optical Radiative Observations, that the correlation between relative dispersion and volume-mean radius changes from positive to negative as volume-mean radius increases. With the new observation, we postulate that the sign of the correlation is determined by whether or not condensation (evaporation) occurs simultaneously with significant new activation (deactivation). The hypothesis is validated by simulations of both an adiabatic cloud parcel model and a parcel model accounting for entrainment-mixing. A new quantity, first bin strength, is introduced to quantify this new observation. Theoretical analysis of truncated gamma and modified gamma size distributions further supports the hypothesis and reconciles the contrasting relationships between relative dispersion and volume-mean radius, including the results in polluted fog observations. The results could shed new light on the so-called “twilight zone” between cloudy and cloud-free air, which in turn affects evaluation of aerosol-cloud interactions and retrieval of aerosol optical depth.

Lu, Chunsong↗
DOE OSTI2025

TRACER-iso Field Campaign Report

The TRACER-iso project took place from June 1 to September 30, 2022, as part of the intensive operational period (IOP) of the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s TRacking Aerosol Convection interactions ExpeRiment (TRACER) at the main project site at the La Porte, Texas, municipal airport. The project sought to use measurements of the stable isotopic composition of water vapor to better understand cloud-aerosol interactions in deep convection in a polluted urban setting.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Water vapor isotopic composition during TRACER IOP

The TRACER-Iso project took place from June 1 to September 30, 2022 as part of the intensive observation period (IOP) of the Tracking Aerosol Convection Interactions (TRACER) project at the main project site at the La Porte, Texas, municipal airport. The project sought to use measurements of the stable isotopic composition of water vapor to better understand cloud-aerosol interactions in deep convection in a polluted urban setting. Water vapor isotopologue and humidity measurements were determined using a Picarro L2130 Water Vapor Isotope Analyzer. The instrument was deployed in the guest van and consists of three main components: a water vapor isotope analyzer, and a Los Gatos Research Water Vapor Isotope Standard Source (WVISS), and a Los Gatos Research Dry Air Source. Ambient air samples were collected through an inlet located about one meter above roof of the shipping container. Samples were then delivered to the analyzer through teflon tubing by use of an external pump to minimize the transport time between the inlet and analyzer. The inlet tubing was surrounded by a Briskheat heat trace and insulating material to ensure ambient air samples did not fall below the dew point and result in condensation. The analyzer uses cavity ringdown spectroscopy to report isotopic ratios of ambient air samples at a frequency of 1 Hz. The calibration unit of the instrument was used in conjunction with the dry air source to periodically measure the δ values of standard waters. It uses a nebulizer to push small water droplets into a hot chamber that vaporizes the water without fractionation. This vapor was then transported to the analyzer using a built-in compressor and the dry air source, which allows each standard with known δ values to be measured at a wide range of humidity values for post-measurement calibration of ambient air samples. There are multiple sources of uncertainty introduced at different stages during the data collection and processing. These include (1) instrument precision, (2) uncertainty in the secondary standards, (3) humidity-correction uncertainty, and (4) VSMOW-SLAP calibration uncertainty. Uncertainty from each step is propagated in quadrature to calculate a total uncertainty of each isotopologue. Uncertainty was determined to be 2.3‰ for δD and 0.4‰ for δ18O.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Characterization of Organosulfates and Organonitrates in Vertically Resolved Aerosols over the Southern Great Plains Field Campaign Report

Aerosol is the largest individual source of uncertainty in assessing the Earth’s radiative balance due to poorly understood aerosol processes and aerosol-cloud interactions. Thus, to constrain aerosol’s climate impacts, it is critical to understand aerosol compositions at high elevations. Organic material accounts for about 20-80% of total aerosol mass in the atmosphere and is known to play a key role in aerosol processes and cloud formation. In prior research, characterization of aerosol molecular composition has been mostly carried out at ground level. In these ground-level measurements, total speciated organosulfates and organonitrates may contribute significantly to organic aerosol mass on the order of 10-40%, most of which are from abundant biogenic volatile organic compounds such as isoprene and monoterpenes. Organosulfates and organonitrates have also been shown to be present in substantial amounts in cloud water, suggesting that they can be transported and/or directly formed at high elevations. On the other hand, the less common and more expensive aircraft studies have performed high-altitude measurements, but were often limited in the number of different altitudes sampled and in sample collection under consistent conditions. Therefore, the vertical distributions of key aerosol components such as organosulfates and organonitrates are not well understood and have not been extensively studied. Nevertheless, it is important to understand how organosulfates and organonitrates in aerosols are distributed, transformed, participate in aqueous-phase processes, and interact with high-altitude clouds.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Enhancements in Cloud Condensation Nuclei Activity From Turbulent Fluctuations in Supersaturation

Abstract The effect of aerosols on the properties of clouds is a large source of uncertainty in predictions of weather and climate. These aerosol‐cloud interactions depend critically on the ability of aerosol particles to form cloud droplets. A challenge in modeling aerosol‐cloud interactions is the representation of interactions between turbulence and cloud microphysics. Turbulent mixing leads to small‐scale fluctuations in water vapor and temperature that are unresolved in large‐scale atmospheric models. To quantify the impact of turbulent fluctuations on cloud condensation nuclei (CCN) activation, we used a high‐resolution Large Eddy Simulation of a convective cloud chamber to drive particle‐based cloud microphysics simulations. We show small‐scale fluctuations strongly impact CCN activity. Once activated, the relatively long timescales of evaporation compared to fluctuations causes droplets to persist in subsaturated regions, which further increases droplet concentrations.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Strategizing emission cuts in China to mitigate short-term warming from clean air policies

Aerosol-cloud interactions remain one of the largest sources of uncertainty in estimates of anthropogenic climate forcing. Reducing aerosols to achieve air quality improvement and climate goals can cause unintended warming due to the weakening of aerosol cooling. Here we investigate the climate impacts of spatially optimized sulfur dioxide (SO 2 ) emission reduction under a carbon-neutral pathway in China. We find that targeting reduction in highly polluted regions in China significantly suppresses the rise in effective radiative forcing due to aerosol-cloud interactions (ERF aci ) during 2020–2060. Owing to the nonlinear aerosol-cloud interaction, the optimized emission reduction strategy limits the regional average increase in ERF aci of more than 0.89 W m −2 to less than 0.13 W m −2 in the short-term future during 2020–2040 and weakens the ERF aci increase by two-thirds in 2060 over China. These findings demonstrate the critical role of targeted emission control in mitigating short-term climate risks while pursuing air quality goals.

Zhu, Yitong [Nanjing Univ. of Information Science ↗
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 OSTI2021

Mass accommodation and gas–particle partitioning in secondary organic aerosols: dependence on diffusivity, volatility, particle-phase reactions, and penetration depth

Abstract. Mass accommodation is an essential process for gas–particle partitioning of organic compounds in secondary organic aerosols (SOA). The mass accommodation coefficient is commonly described as the probability of a gas molecule colliding with the surface to enter the particle phase. It is often applied, however, without specifying if and how deep a molecule has to penetrate beneath the surface to be regarded as being incorporated into the condensed phase (adsorption vs. absorption). While this aspect is usually not critical for liquid particles with rapid surface–bulk exchange, it can be important for viscous semi-solid or glassy solid particles to distinguish and resolve the kinetics of accommodation at the surface, transfer across the gas–particle interface, and further transport into the particle bulk. For this purpose, we introduce a novel parameter: an effective mass accommodation coefficient αeff that depends on penetration depth and is a function of surface accommodation coefficient, volatility, bulk diffusivity, and particle-phase reaction rate coefficient. Application of αeff in the traditional Fuchs–Sutugin approximation of mass-transport kinetics at the gas–particle interface yields SOA partitioning results that are consistent with a detailed kinetic multilayer model (kinetic multilayer model of gas–particle interactions in aerosols and clouds, KM-GAP; Shiraiwa et al., 2012) and two-film model solutions (Model for Simulating Aerosol Interactions and Chemistry, MOSAIC; Zaveri et al., 2014) but deviate substantially from earlier modeling approaches not considering the influence of penetration depth and related parameters. For highly viscous or semi-solid particles, we show that the effective mass accommodation coefficient remains similar to the surface accommodation coefficient in the case of low-volatility compounds, whereas it can decrease by several orders of magnitude in the case of semi-volatile compounds. Such effects can explain apparent inconsistencies between earlier studies deriving mass accommodation coefficients from experimental data or from molecular dynamics simulations. Our findings challenge the approach of traditional SOA models using the Fuchs–Sutugin approximation of mass transfer kinetics with a fixed mass accommodation coefficient, regardless of particle phase state and penetration depth. The effective mass accommodation coefficient introduced in this study provides an efficient new way of accounting for the influence of volatility, diffusivity, and particle-phase reactions on SOA partitioning in process models as well as in regional and global air quality models. While kinetic limitations may not be critical for partitioning into liquid SOA particles in the planetary boundary layer (PBL), the effects are likely important for amorphous semi-solid or glassy SOA in the free and upper troposphere (FT–UT) as well as in the PBL at low relative humidity and low temperature.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

NSA Site Science: Use of ARM Observations from Northern Alaska to Evaluate and Improve Prediction Capabilities

The Arctic is warming at a rate nearly double that of the rest of the planet, leading to profound changes in atmospheric, oceanic, and ice processes. The U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility has played a significant role in Arctic research, operating observatories in Alaska's North Slope for over 25 years. These observatories provide a rich, and wide-reaching dataset that offers insight into atmospheric processes in northern Alaska. This report details the results of a nine-year research project (2015–2024) supported by the DOE Atmospheric Systems Research (ASR) program, that leverages data from ARM’s deployment of observing facilities at Utqiaġvik (known as the North Slope of Alaska, or NSA, site) and Oliktok Point, Alaska. The project was conducted in two phases: - Phase 1 (2015–2019): Focused on understanding key atmospheric processes at Oliktok Point, including cloud formation, high-latitude precipitation, aerosol-cloud interactions, and cloud properties. - Phase 2 (2019–2024): Extended the research to the broader North Slope region, using data from both Oliktok Point and Utqiaġvik. Topics explored included surface energy budgets, atmospheric stability, ice nucleation processes, and microphysics in Arctic clouds. The project resulted in numerous research products, including 50 peer-reviewed publications and dissertations, 169 presentations, and 10 data products. These products cover a variety of topics, including: - Cloud Macro- and Microphysical Properties: Arctic clouds play a crucial role in energy transfer, and accurate representation in models is critical. The study explored cloud transitions, ice crystal shapes, and dual-wavelength radar data to understand ice crystal habits and size distributions. - Aerosol Properties and Processes: The team examined aerosol sources in the Arctic, including industrial emissions and natural sources. Observations showed significant spatial gradients in aerosol concentrations due to human activities and wildfire smoke. The influence of aerosols on cloud formation and the surface energy budget was also assessed. - Aerosol-Cloud Interactions: Research revealed that aerosols might suppress cloud ice production, affecting cloud radiative forcing and precipitation. The impact of local industrial emissions on cloud properties was also investigated. - Contextualizing the North Slope of Alaska in the context of the broader Arctic: To understand broader trends, the project evaluated large-scale circulation patterns and the influence of weather systems on the Arctic. Studies indicated that large-scale processes play a significant role in temperature patterns and the timing of snowmelt. - Advancing ARM Observational and Modeling Capabilities: The project developed new radar data products and advanced measurement techniques, including clutter mitigation and drizzle detection. Uncrewed aerial systems (UAS) and tethered balloon systems (TBS) were deployed to gather detailed atmospheric data. Additionally, the project supported 10 early career scientists, providing training and mentorship to undergraduate interns, graduate students, postdoctoral researchers, and early career researchers. These efforts contributed to the advancement of ARM research capabilities and fostered a new generation of scientists skilled in Arctic atmospheric research. Ultimately, this ASR-supported project has provided valuable insights into Arctic atmospheric processes and their broader climate implications. Recommendations for future work include continuing support for long-term observing at Arctic locations to foster additional research, further exploration of aerosol-cloud interactions and the potential impacts of enhanced industrialization of the Arctic, and expanded use of uncrewed systems to gather data in this remote and harsh environment. Additionally, the data products developed by this work, and the data products developed through the ARM infrastructure, leave a treasure-trove of additional information that should be explored for many years to come to gain additional insight into physical processes in the Arctic atmosphere that drive the rapid changes occurring in at high latitudes and their global impact.

58 GEOSCIENCES↗
DOE OSTI2023

The Dichotomy of Wet and Dry Trends Over India by Aerosol Indirect Effects in CMIP5 Models

Abstract Aerosol‐cloud interactions, also known as aerosol indirect effect (AIE), substantially impact rainfall frequency and intensity. Here, we analyze NEX‐GDDP, a multimodel ensemble of high‐resolution (0.25°) historical simulations and future projections statistically downscaled from 21 CMIP5 models, to quantify the importance of AIE on extreme climate indices, specifically consecutive dry days (CDD), consecutive wet days (CWD), and simple daily intensity index (SDII). The 21 NEX‐GDDP CMIP5 models are classified into models with reliable (REM) and unreliable (UREM) monsoon climate simulated over India based on their simulations of the climate indices. The REM group is further decomposed based on whether the models represent only the direct (REM ADE ) or the direct and indirect (REM ALL ) aerosol effects. Compared to REM ADE , including all aerosol effects significantly improves the model skills in simulating the observed historical trends of all three climate indices over India. Specifically, AIE enhances dry days and reduces wet days in India in the historical period, consistent with the observed changes. However, by the middle and end of the 21st century, there is a relative decrease in dry days and an increase in wet days and precipitation intensity. Moreover, the REM ALL simulated future CWD and CDD changes are mostly opposite to those in REM ADE , indicating the substantial role of AIE in the future projection of dry and wet climates. These findings underscore the crucial role of AIE in future projections of the Indian hydroclimate and motivate efforts to accurately represent AIE in climate models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Drivers of Cloud Condensation Nuclei in the Eastern North Atlantic as Observed at the ARM Site

Abstract Seven years of data collected at the Atmospheric Radiation Measurement's Eastern North Atlantic (ENA) site are analyzed to understand the controls of Cloud Condensation Nuclei (CCN) concentrations in the region. Day‐night differences in the aerosol data as segregated by wind direction demonstrate the aerosol observations to be impacted by local emissions when the wind direction (wdir) is between 90° and 310° (measured clockwise from the North where air is coming from). Data collected during marine conditions (wdir <90° or wdir >310°) show the CCN concentrations to be higher in the summer months as compared to the winter months. CCN budget analysis revealed advection and precipitation scavenging being primarily responsible for modulating the CCN concentrations at the site on monthly timescales, with rain rates driving the precipitation scavenging term. High (greater than 75th percentile) and low (lower than 25th percentile) CCN events were identified for each month to characterize the sub‐monthly variability of CCN concentrations. Low CCN events had thicker clouds, stronger rain rates, and lower reanalysis reported free‐tropospheric aerosol pseudo number concentration at the ENA site as compared to the high CCN events. Analysis of satellite data of air‐parcels 48 hr prior to their arrival at the ENA site demonstrated the air parcels during low CCN events to encounter higher cloudiness, stronger rain rates, and higher cloud top heights as compared to the high CCN events. The results presented herein provide key constraints for model evaluation studies and climatological studies conducted at the ENA site.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

62°S Witnesses the Transition of Boundary Layer Marine Aerosol Pattern Over the Southern Ocean (50°S–68°S, 63°E– 150°E) During the Spring and Summer: Results From MARCUS (I)

The Atmospheric Radiation Measurement Mobile Facility-2 was installed onboard the research vessel Aurora Australis to measure aerosol properties during the 2017-2018 Measurement of Aerosols, Radiation, and CloUds over the pristine Southern ocean (MARCUS) Experiment, providing unique data on aerosols latitudinal and seasonal variation, including south of 60 degrees S where previous observations are scarce. Data from a Cloud Condensation Nuclei (CCN) counter and Ultra-High-Sensitivity Aerosol Spectrometer show that both the number concentration (N-CCN) and size distribution of CCN-active aerosols, with diameters (D) between 60 nm < D < 1,000 nm are different over the North Southern Ocean (NSO) (50 degrees S-60 degrees S) and the South Southern Ocean (SSO) (62 degrees S-68 degrees S). The average NSO N-CCN at 0.2% and 0.5% supersaturation were 28% and 49% less than that over the SSO. This increase of CCN over the SSO is caused by the increase of aerosols with 60 nm < D < 200 nm, consistent with calculations of Aerosol Scattering Angstrom Exponents derived from a nephelometer. Aerosol hygroscopicity growth factor measured by the Hygroscopic Tandem Differential Mobility Analyzer stayed close to 1.41 for aerosols with 50 nm < D < 250 nm over the SSO, but increased from 1.30 to 1.67 over the NSO, indicating different chemical compositions. Both CCN and Ice Nucleating Particles (INPs) showed a stronger variation with season than with latitude. The variation of heat-labile and presumably proteinacous INPs suggests an increase of ice nucleating-active microbes in summer.

Niu, Qing↗
DOE OSTI2022

A perspective on iron (Fe) in the atmosphere: air quality, climate, and the ocean

As scientists engage in research motivated by climate change and the impacts of pollution on air, water, and human health, we increasingly recognize the need for the scientific community to improve communication and knowledge exchange across disciplines to address pressing and outstanding research questions holistically. Our professional paths have crossed because our research activities focus on the chemical reactivity of Fe-containing minerals in air and water, and at the air-sea interface. (Photo)chemical reactions driven by Fe can take place at the surface of the particles/droplets or within the condensed phase. The extent and rates of these reactions are influenced by water content and biogeochemical activity ubiquitous in these systems. One of these reactions is the production of reactive oxygen species (ROS) that cause damage to respiratory organs. Another is that the reactivity of Fe and organics in aerosol particles alter surficial physicochemical properties that impact aerosol-radiation and aerosol–cloud interactions. Also, upon deposition, aerosol particles influence ocean biogeochemical processes because micronutrients such as Fe or toxic elements such as copper become bioavailable. We provide a perspective on these topics and future research directions on the reactivity of Fe in atmospheric aerosol systems, from sources to short- and long-term impacts at the sinks with emphasis on needs to enhance the predictive power of atmospheric and ocean models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

TRACER Carbonaceous Aerosols Thrust – University of California, Davis Field Campaign Report

The broader U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s TRacking Aerosol Convection interactions ExpeRiment (TRACER) campaign aims to increase our understanding of convective cloud life cycles and aerosol-convection interactions. Our TRACER Carbonaceous Aerosols Thrust-University of California, Davis (TRACER-CAT-UCDavis) study complemented these broader aims by characterizing and quantifying the optical properties and composition of carbonaceous aerosols during part of the TRACER intensive sampling period (July 1- July 31, 2022) at the first ARM Mobile Facility (AMF1) main site (M1) in La Porte, Texas. Our measurements complemented the suite of instrumentation already provided by the AMF1, expanding the capabilities through deployment of unique, state-of-the-science instrumentation. The instrumentation included: (i) two cavity-attenuated phase shift spectroscopy single-scatter albedo (CAPS-SSA) instruments operating at 530 nm and 630 nm, and that were modified to characterize particle light absorption, extinction, and scattering at elevated humidities; (ii) the UC Davis dual-wavelength cavity ringdown-photoacoustic spectrometer (CRD-PAS), which characterizes dry particle extinction and absorption at 405 nm and 532 nm; (iii) a soot particle aerosol mass spectrometer (SP-AMS) that operated in “laser only” mode that characterized the size-dependent compositions of black carbon (BC)-containing particles; (v) a thermal denuder, to remove coatings on particles; and (vi) a scanning electrical mobility sizer (SEMS), to characterize particle mobility diameters from 10-1300 nm. Our measurements occurred alongside complementary observations made by Los Alamos National Laboratory (LANL) during the TRACER-CAT-LANL study, including a humidified CAPS-SSA instrument operating at 450 nm. Our primary scientific interest is in understanding the relationship between particle composition and light absorption, with a particular focus on the influence of water uptake. While it is known that coatings on BC can enhance absorption, the extent to which this occurs in the atmosphere and the specific role that water plays as a coating remain unclear. The TRACER-CAT-UCDavis measurements were made with near-complete coverage for the CRD-PAS, SP-AMS, and SEMS throughout the intensive period. The UC Davis humidified CAPS-SSA instruments had significant challenges with operation owing to the demanding conditions (large temperature fluctuations, high humidity), exacerbated by supply chain issues that delayed resolution of these challenges. However, the humidified CAPS-SSA instrument operated by LANL operated throughout the intensive period with near-complete coverage. The dry light extinction measurements from the CRD-PAS measurements and the LANL CAPS-SSA exhibited a good correlation, although the CAPS-SSA systematically measured greater extinction values than expected. While all instruments, with the exception of an aerodynamic particle sizer (APS), measured behind a common particulate matter (PM)2.5 μm cyclone, the greater extinction measured by the LANL CAPS-SSA compared to the CRD-PAS may have resulted from different losses of larger particles in the sampling lines from the cyclone to the instruments; the tubing length was shorter from the cyclone to the LANL CAPS-SSA, consistent with this idea. A summary of the TRACER-CAT-UCDavis measurements, along with some of the TRACER-CAT-LANL measurements, are shown in the figure below. Notably, there were periods when the contributions of presumed dust were substantial and even dominated the observed light extinction and absorption. Also, there was a clear shift in the behavior of submicron particles from before July 16, 2022 to after, with the prior period exhibiting regular episodes of new particle formation and the latter period exhibiting rapid variations in the concentrations of small particles.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Dry and warm conditions in Australia exacerbated by aerosol reduction in China

A substantial decline in anthropogenic aerosols in China has been observed since the initiation of clean air actions in 2013. This study reveals a linkage between aerosol reductions in China and drier and warmer conditions in Australia. Aerosol decline in China trigger alterations in temperature and pressure gradients between the two hemispheres, leading to intensified outflow from Asia towards the South Indian Ocean, strengthening the Southern Indian Subtropical High and its related Southern Trade Winds. Consequently, this atmospheric pattern results in a moisture divergence over Australia. The reduction in surface moisture further results in more surface energy being converted into sensible heat instead of evaporating as latent heat, warming the near-surface air. The intensified dry and warm climate conditions further cause the increase in wildfire risks during fire seasons in Australia. Our study illuminates the potential impact of distant aerosols on precipitation and temperature variations in Australia, offering valuable insights for drought and wildfire risk mitigation in Australia.

aerosol-cloud interaction↗