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32 records · Page 2

Rapid evolution of aerosol particles and their optical properties downwind of wildfires in the western US

Abstract. During the first phase of the Biomass Burn Operational Project (BBOP) field campaign, conducted in the Pacific Northwest, the DOE G-1 aircraft was used to follow the time evolution of wildfire smoke from near the point of emission to locations 2–3.5 h downwind. In nine flights we made repeated transects of wildfire plumes at varying downwind distances and could thereby follow the plume's time evolution. On average there was little change in dilution-normalized aerosol mass concentration as a function of downwind distance. This consistency hides a dynamic system in which primary aerosol particles are evaporating and secondary ones condensing. Organic aerosol is oxidized as a result. On all transects more than 90 % of aerosol is organic. In freshly emitted smoke aerosol, NH4+ is approximately equivalent to NO3. After 2 h of daytime aging, NH4+ increased and is approximately equivalent to the sum of Cl, SO42, and NO3. Particle size increased with downwind distance, causing particles to be more efficient scatters. Averaged over nine flights, mass scattering efficiency (MSE) increased in ∼ 2 h by 56 % and doubled in one flight. Mechanisms for redistributing mass from small to large particles are discussed. Coagulation is effective at moving aerosol from the Aitken to accumulation modes but yields only a minor increase in MSE. As absorption remained nearly constant with age, the time evolution of single scatter albedo was controlled by age-dependent scattering. Near-fire aerosol had a single scatter albedo (SSA) of 0.8–0.9. After 1 to 2 h of aging SSAs were typically 0.9 and greater. Assuming global-average surface and atmospheric conditions, the observed age dependence in SSA would change the direct radiative effect of a wildfire plume from near zero near the fire to a cooling effect downwind.

54 ENVIRONMENTAL SCIENCES↗

A full year of aerosol size distribution data from the central Arctic under an extreme positive Arctic Oscillation: insights from the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition

Abstract. The Arctic environment is rapidly changing due to accelerated warming in the region. The warming trend is driving a decline in sea ice extent, which thereby enhances feedback loops in the surface energy budget in the Arctic. Arctic aerosols play an important role in the radiative balance and hence the climate response in the region, yet direct observations of aerosols over the Arctic Ocean are limited. In this study, we investigate the annual cycle in the aerosol particle number size distribution (PNSD), particle number concentration (PNC), and black carbon (BC) mass concentration in the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition. This is the first continuous, year-long data set of aerosol PNSD ever collected over the sea ice in the central Arctic Ocean. We use a k-means cluster analysis, FLEXPART simulations, and inverse modeling to evaluate seasonal patterns and the influence of different source regions on the Arctic aerosol population. Furthermore, we compare the aerosol observations to land-based sites across the Arctic, using both long-term measurements and observations during the year of the MOSAiC expedition (2019–2020), to investigate interannual variability and to give context to the aerosol characteristics from within the central Arctic. Our analysis identifies that, overall, the central Arctic exhibits typical seasonal patterns of aerosols, including anthropogenic influence from Arctic haze in winter and secondary aerosol processes in summer. The seasonal pattern corresponds to the global radiation, surface air temperature, and timing of sea ice melting/freezing, which drive changes in transport patterns and secondary aerosol processes. In winter, the Norilsk region in Russia/Siberia was the dominant source of Arctic haze signals in the PNSD and BC observations, which contributed to higher accumulation-mode PNC and BC mass concentrations in the central Arctic than at land-based observatories. We also show that the wintertime Arctic Oscillation (AO) phenomenon, which was reported to achieve a record-breaking positive phase during January–March 2020, explains the unusual timing and magnitude of Arctic haze across the Arctic region compared to longer-term observations. In summer, the aerosol PNCs of the nucleation and Aitken modes are enhanced; however, concentrations were notably lower in the central Arctic over the ice pack than at land-based sites further south. The analysis presented herein provides a current snapshot of Arctic aerosol processes in an environment that is characterized by rapid changes, which will be crucial for improving climate model predictions, understanding linkages between different environmental processes, and investigating the impacts of climate change in future Arctic aerosol studies.

54 ENVIRONMENTAL SCIENCES↗

Final report: Insights from ARM observations into aerosol processing and transport by extratropical cyclones and aerosol effects on cyclone clouds

This project advanced understanding of aerosol–cloud interactions in extratropical cyclones using observations from the Atmospheric Radiation Measurement (ARM) Eastern North Atlantic (ENA) observatory and ACE-ENA field campaigns, along with satellite datasets and numerical modeling. We have quantified the susceptibility of frontal clouds to aerosols, showing that this susceptibility is similar to that in non-frontal clouds despite substantial (factor 2) differences in droplet concentrations between these cloud types, and also significant differences in cloud albedo. A key finding was that Aitken-mode (here, 60-100nm diameter) aerosols play a disproportionately important role in droplet activation in frontal clouds, and concentrations of these particles are frequently strongly biased in climate models. Activation of aerosols depends strongly on updraft speeds, and via collaboration with Argonne National Laboratory we contributed to quantifying these better with the ARM radar wind profiler at the ENA site. Our studies in the North Atlantic have analogs in the Southern Ocean, and to draw these out we examined data from the MARCUS and SOCRATES field campaigns. We identified new particle formation within extratropical cyclones as a potentially important source of cloud condensation nuclei in these pristine marine environments. By combining ARM observations with perturbed parameter ensemble simulations, we demonstrated that surface observations can effectively constrain aerosol–cloud adjustments and reduce uncertainty in simulated cloud liquid water path responses by approximately 15%, yielding stronger constraints on historical aerosol cooling effects. The work further established precipitation processes as a dominant control on aerosol–cloud interactions and Earth system predictability.

Gordon, Hamish [Department of Chemical Engineering↗

Tethered Balloon Observations of Vertically Resolved Aerosol Size Distributions during the U.S. DOE ARM CoURAGE and BNF Campaigns

This dataset contains vertically resolved aerosol particle number size distributions measured using a miniature Scanning Electrical Mobility Spectrometer (mSEMS) deployed aboard the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) Tethered Balloon System (TBS) during the 2025 Coast-Urban-Rural Atmospheric Gradient Experiment (CoURAGE) and Bankhead National Forest (BNF) field campaigns. The mSEMS measured aerosol size distributions over approximately 10–300 nm during repeated TBS vertical profiles through the atmospheric boundary layer. The dataset provides measurements of particle number size distributions as a function of particle diameter, altitude, and time and supports investigation of aerosol vertical structure, elevated ultrafine and Aitken-mode particle layers, boundary-layer evolution, and residual-layer processes.

ARM↗

Properties and Controlling Processes of Aerosol and Cloud Condensation Nuclei in Marine Boundary Layer Over Eastern North Atlantic (Final Report)

Remote marine low cloud systems have large spatial and temporal coverages. Because of their relatively low optical thickness and background aerosol concentrations, marine low clouds are particularly susceptible to perturbations in aerosols associated with anthropogenic emissions. Recent studies show that a large fraction of the global aerosol indirect forcing can be attributed to changes in marine low clouds, despite their relatively long distance from most anthropogenic sources. Currently, there remain large uncertainties in the magnitude of the global aerosol indirect radiative forcing. One major contribution to this large uncertainty derives from poor understanding of the aerosols under natural conditions, the perturbation by anthropogenic emissions, and the processes that drive them. In this project, we took advantage of the comprehensive, multi-dimensional characterization of meteorological parameters, trace gases, aerosol, cloud, and drizzle fields during the Aerosol and Cloud Experiments in Eastern North Atlantic (ACE-ENA) and the long-term measurements at the Atmospheric Radiation Measurement (ARM) Eastern North Atlantic (ENA) site on Graciosa Island. By synergistically combining in situ measurements, remote sensing retrievals, and model simulations, we quantified aerosol properties in the ENA, their vertical profiles, and variations with season, synoptic state, and airmass. We investigated key aerosol processes, including entrainment of free troposphere aerosol into marine boundary layer, new particle formation, growth of Aitken mode particles, and the influences of these processes on the cloud condensation nuclei (CCN) population in marine boundary layer. The representation of key aerosol processes in the Energy Exascale Earth System Model (E3SM) was evaluated using the observations. This project has led to 26 publications, which are listed at the end of this report.

54 ENVIRONMENTAL SCIENCES↗

Aerosol‐Correlated Cloud Activation for Clean Conditions in the Tropical Atlantic Boundary Layer During LASIC

Abstract Aerosol measurements during the DOE ARM Layered Atlantic Smoke Interactions with Clouds (LASIC) campaign were used to quantify the differences between clean and smoky cloud condensation nuclei (CCN) budgets. Accumulation‐mode particles accounted for ∼70% of CCN at supersaturations <0.3% in clean and smoky conditions. Aitken‐mode particles contributed <20% and sea‐spray‐mode particles <10% at supersaturations <0.3%, but at supersaturations >0.3% Aitken particles contributions increased to 30%–40% of clean CCN. For clean conditions, the Hoppel minimum diameter was correlated to the accumulation‐mode number concentration, indicating aerosol‐correlated cloud activation was controlling the lower diameter cutoff for which particles serve as CCN. For smoky conditions, the contributions of Aitken particles increase and the correlation of cloud activation to accumulation‐mode particles is masked by the lower‐hygroscopicity smoke. These results provide the first multi‐month in situ quantitative constraints on the role of aerosol number size distributions in controlling cloud activation in the tropical Atlantic boundary layer.

54 ENVIRONMENTAL SCIENCES↗

Particle-Phase Diffusion Modulates Partitioning of Semivolatile Organic Compounds to Aged Secondary Organic Aerosol

The diffusivity of semivolatile organic compounds (SVOCs) in the bulk particle phase of a viscous atmospheric secondary organic aerosol (SOA) can have a profound impact on aerosol growth and size distribution dynamics. Here, we investigate the bulk diffusivity of SVOCs formed from photo-oxidation of isoprene as they partition to a bimodal aerosol consisting of an Aitken (potassium sulfate) and accumulation mode (aged α-pinene SOA) particles as a function of relative humidity (RH). The model analysis of the observed size distribution evolution shows that liquid-like diffusion coefficient values of D b > 10 –10 cm 2 s –1 fail to explain the growth of the Aitken mode. Instead, much lower values of Db between 2.5 × 10 –15 cm 2 s –1 at 32% RH and 8 × 10 –15 cm 2 s –1 at 82% RH were needed to successfully reproduce the growth of both modes. The diffusivity within the aged α-pinene SOA remains appreciably slow even at 80% RH, resulting in hindered partitioning of SVOCs to large viscous particles and allowing smaller and relatively less viscous particles to effectively absorb the available SVOCs and grow much faster than would be possible otherwise. Our results have important implications for modeling SOA formation and growth in the ambient atmosphere.

54 ENVIRONMENTAL SCIENCES↗

Identifying a regional aerosol baseline in the eastern North Atlantic using collocated measurements and a mathematical algorithm to mask high-submicron-number-concentration aerosol events

Abstract. High-time-resolution measurements of in situ aerosol and cloud properties provide the ability to study regional atmospheric processes that occur on timescales of minutes to hours. However, one limitation to this approach is that continuous measurements often include periods when the data collected are not representative of the regional aerosol. Even at remote locations, submicron aerosols are pervasive in the ambient atmosphere with many sources. Therefore, periods dominated by local aerosol should be identified before conducting subsequent analyses to understand aerosol regional processes and aerosol–cloud interactions. Here, we present a novel method to validate the identification of regional baseline aerosol data by applying a mathematical algorithm to the data collected at the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility in the eastern North Atlantic (ENA). The ENA central facility (C1) includes an aerosol observing system (AOS) for the measurement of aerosol physical, optical, and chemical properties at time resolutions from seconds to minutes. A second temporary supplementary facility (S1), located ∼0.75 km from C1, was deployed for ∼1 year during the Aerosol and Cloud Experiments (ACE-ENA) campaign in 2017. First, we investigate the local aerosol at both locations. We associate periods of high submicron number concentration (Ntot) in the fine-mode condensation particle counter (CPC) and size distributions from the Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) as a function of wind direction using a meteorology sensor with local sources. Elevated concentrations of Aitken-mode (< 100 nm diameter) particles were observed in correspondence with the wind directions associated with airport operations. At ENA, the Graciosa Airport and its associated activities were found to be the main sources of high-concentration aerosol events at ENA, causing peaks in 1 min Ntot that exceeded 8000 and 10 000 cm−3 at C1, in summer and winter, respectively, and 5000 cm−3 at S1 in summer. Periods with high Ntot not associated with these wind directions were also observed. As a result, the diverse local sources at ENA yielded a poor relationship between Ntot measurements collected at C1 and S1 (R2=0.03 with a slope =0.05±0.001). As a first approach to mask these events, the time periods when the wind direction was associated with the airport operations (west to northwest and southeast to south at C1 and east to south at S1) were applied. The meteorological masks removed 38.9 % of the data at C1 and 43.4 % at S1, and they did not significantly improve the relationship between the two sites (R2=0.18 with a slope =0.06±0.001). Due to the complexity of high-Ntot events observed at ENA, we develop and validate a mathematical ENA Aerosol Mask (ENA-AM) to identify high-Ntot events using 1 min resolution data from the AOS CPC at C1 and S1. After its parameterization and application, ENA-AM generated a high correlation between Ntot in the summer at C1 and S1 (R2=0.87 with a slope =0.84±0.001). We identified the regional baseline at ENA to be 428±228 cm−3 in the summer and 346±223 cm−3 in the winter. Lastly, we compared masked measurements from the AOS with the ARM Aerial Facility (AAF) during flights over C1 in the summer to understand submicron aerosol vertical mixing over C1. The high correlation (R2=0.71 with a slope of 1.04±0.01) observed between C1 and the AAF Ntot collected within an area of 10 km surrounding ENA and at altitudes < 500 m indicated that the submicron aerosol at ENA was well mixed within the first 500 m of the marine boundary layer during the month of July during ACE-ENA. Our novel method for determining a regional aerosol baseline at ENA can be applied to other time periods and at other locations with validation by a secondary site or additional collocated measurements.

54 ENVIRONMENTAL SCIENCES↗

Intercomparison and Evaluation of Global Aerosol Microphysical Properties Among Aerocom Models of a Range of Complexity

Many of the next generation of global climate models will include aerosol schemes which explicitly simulate the microphysical processes that determine the particle size distribution. These models enable aerosol optical properties and cloud condensation nuclei (CCN) concentrations to be determined by fundamental aerosol processes, which should lead to a more physically based simulation of aerosol direct and indirect radiative forcings. This study examines the global variation in particle size distribution simulated by 12 global aerosol microphysics models to quantify model diversity and to identify any common biases against observations. Evaluation against size distribution measurements from a new European network of aerosol supersites shows that the mean model agrees quite well with the observations at many sites on the annual mean, but there are some seasonal biases common to many sites. In particular, at many of these European sites, the accumulation mode number concentration is biased low during winter and Aitken mode concentrations tend to be overestimated in winter and underestimated in summer. At high northern latitudes, the models strongly underpredict Aitken and accumulation particle concentrations compared to the measurements, consistent with previous studies that have highlighted the poor performance of global aerosol models in the Arctic. In the marine boundary layer, the models capture the observed meridional variation in the size distribution, which is dominated by the Aitken mode at high latitudes, with an increasing concentration of accumulation particles with decreasing latitude. Considering vertical profiles, the models reproduce the observed peak in total particle concentrations in the upper troposphere due to new particle formation, although modelled peak concentrations tend to be biased high over Europe. Overall, the multimodel- mean data set simulates the global variation of the particle size distribution with a good degree of skill, suggesting that most of the individual global aerosol microphysics models are performing well, although the large model diversity indicates that some models are in poor agreement with the observations. Further work is required to better constrain size-resolved primary and secondary particle number sources, and an improved understanding of nucleation an growth (e.g. the role of nitrate and secondary organics) will improve the fidelity of simulated particle size distributions.

Cloud physics↗

The Messy Aerosol Submodel MADE3 (v2.0b): Description and a Box Model Test

We introduce MADE3 (Modal Aerosol Dynamics model for Europe, adapted for global applications, 3rd generation), an aerosol dynamics submodel for application within the MESSy framework (Modular Earth Submodel System). MADE3 builds on the predecessor aerosol submodels MADE and MADE-in. Its main new features are the explicit representation of coarse particle interactions both with other particles and with condensable gases, and the inclusion of hydrochloric acid (HCl)chloride (Cl) partitioning between the gas and condensed phases. The aerosol size distribution is represented in the new submodel as a superposition of nine lognormal modes: one for fully soluble particles, one for insoluble particles, and one for mixed particles in each of three size ranges (Aitken, accumulation, and coarse mode size ranges). In order to assess the performance of MADE3 we compare it to its predecessor MADE and to the much more detailed particle-resolved aerosol model PartMC-MOSAIC in a box model simulation of an idealized marine boundary layer test case. MADE3 and MADE results are very similar, except in the coarse mode, where the aerosol is dominated by sea spray particles. Cl is reduced in MADE3 with respect to MADE due to the HClCl partitioning that leads to Cl removal from the sea spray aerosol in our test case. Additionally, aerosol nitrate concentration is higher in MADE3 due to the condensation of nitric acid on coarse particles. MADE3 and PartMC- MOSAIC show substantial differences in the fine particle size distributions (sizes about 2 micrometers) that could be relevant when simulating climate effects on a global scale. Nevertheless, the agreement between MADE3 and PartMC-MOSAIC is very good when it comes to coarse particle size distribution, and also in terms of aerosol composition. Considering these results and the well-established ability of MADE in reproducing observed aerosol loadings and composition, MADE3 seems suitable for application within a global model.

Mixing state↗

Revisiting particle dry deposition and its role in radiative effect estimates

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

54 ENVIRONMENTAL SCIENCES↗

The Shortwave Radiative Flux Response to an Injection of Sea Salt Aerosols in the Gulf of Mexico

We report marine cloud brightening (MCB) has been proposed as a potential means of geoengineering the climate, temporarily providing cooling to offset some of the effects of climate change. Marine sky brightening (MSB), involving the direct scattering of sunlight from sea salt injection into the marine boundary layer, has been proposed as an additional geoengineering method that could work in areas that are not regularly cloudy. Here, we use a regional atmospheric model to simulate MCB and MSB over the Gulf of Mexico and nearby land, a highly populated and economically important region that is not characterized by persistent marine stratocumulus cloud cover. Injection of sea salt in the Aitken mode from a region in the central Gulf of Mexico equivalent to 10.8 Tg yr -1 produces an upwards 8.4 W m -2 radiative flux change across the region at the top of the atmosphere, largely due to cloud property changes. Comparatively, a similar mass injection in the accumulation mode produces a 3.1 W m -2 radiative flux change driven primarily by direct scattering. Injection of even larger particles produces a much smaller radiative flux change. Shortwave flux changes due to clouds are largely driven by an increase in cloud droplet number concentration and an increase in cloud liquid water path (each contributing about 45% to the flux change), with a much lower contribution from cloud fraction changes (10%).

54 ENVIRONMENTAL SCIENCES↗

Solid organic-coated ammonium sulfate particles at high relative humidity in the summertime Arctic atmosphere

The ability of atmospheric aerosols to impact climate through water uptake and cloud formation is fundamentally determined by the size, composition, and phase (liquid, semisolid, or solid) of individual particles. Particle phase is dependent on atmospheric conditions (relative humidity and temperature) and chemical composition and, importantly, solid particles can inhibit the uptake of water and other trace gases, even under humid conditions. Particles composed primarily of ammonium sulfate are presumed to be liquid at the relative humidities (67 to 98%) and temperatures (–2 to 4 °C) of the summertime Arctic. Under these atmospheric conditions, we report the observation of solid organic-coated ammonium sulfate particles representing 30% of particles, by number, in a key size range (<0.2 µm) for cloud activation within marine air masses from the Arctic Ocean at Utqiagvik, AK. The composition and size of the observed particles are consistent with recent Arctic modeling and observational results showing new particle formation and growth from dimethylsulfide oxidation to form sulfuric acid, reaction with ammonia, and condensation of marine biogenic sulfate and highly oxygenated organic molecules. Aqueous sulfate particles typically undergo efflorescence and solidify at relative humidities of less than 34%. Therefore, the observed solid phase is hypothesized to occur from contact efflorescence during collision of a newly formed Aitken mode sulfate particle with an organic-coated ammonium sulfate particle. With declining sea ice in the warming Arctic, this particle source is expected to increase with increasing open water and marine biogenic emissions.

54 ENVIRONMENTAL SCIENCES↗

Sources, Transport and Visibility Impact of Ambient Submicrometer Particle Size Distributions in an Urban Area of Central Taiwan

This study applied positive matrix factorization (PMF) to identify the sources of size-resolved submicrometer (10–1000 nm) particles and quantify their contributions to impaired visibility based on the particle number size distributions (PNSDs), aerosol light extinction (b p ), air pollutants (PM 10 , PM 2.5 , SO 2 , O 3 , and NO), and meteorological parameters (temperature, relative humidity, wind speed, wind direction, and ultraviolet index) measured hourly over an urban basin in central Taiwan between 2017 and 2021. The transport of source-specific PNSDs was evaluated with wind and back trajectory analyses. The PMF revealed six sources to the total particle number (TPN), surface (TPS), volume (TPV), and b p . Factor 1 (F1), the key contributor to TPN (35.0 %), represented nucleation (<25 nm) particles associated with fresh traffic emission and secondary new particle formation, which were transported from the west-southwest by stronger winds (>2.2 m s -1 ). F2 represented the large Aitken (50–100 nm) particles transported regionally via northerly winds, whereas F3 represented large accumulation (300–1000 nm) particles, which showed elevated concentrations under stagnant conditions (<1.1 m s −1 ). F4 represented small Aitken (25–50 nm) particles arising from the growth and transport of the nucleation particles (F1) via west-southwesterly winds. F5 represented large Aitken particles originating from combustion-related SO 2 sources and carried by west-northwesterly winds. F6 represented small accumulation (100–300 nm) particles emitted both by local sources and by the remote SO 2 sources found for F5. Overall, large accumulation particles (F3) played the greatest role in determining the TPV (66.4 %) and TPS (34.8 %), and their contribution to bp increased markedly from 17.3 % to 40.7 % as visibility decreased, indicating that TPV and TPS are better metrics than TPN for estimating b p . Furthermore, slow-moving air masses—and therefore stagnant conditions—facilitate the build-up of accumulation mode particles (F3 + F6), resulting in the poorest visibility.

source apportionment↗