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Creators/Authors contains: "Sheesley, Rebecca J"

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  1. Rapid warming is likely increasing primary production and wildfire occurrence in the Arctic. Projected changes in the abundance and composition of carbonaceous aerosols during the summer are likely to impact atmospheric chemistry and climate, but our understanding of these processes is limited by sparse observations. Here, we characterize carbonaceous aerosol at two field sites, Toolik Field Station in the Interior and the Atmospheric Radiation Measurement facility at Utqiaġvik on the Arctic coast of Alaska, USA, through the summers of 2022 and 2023. We estimated particulate matter ≤2.5 micrometers (PM2.5) and particulate matter ≤10 micrometers (PM10) using laser light scattering (PurpleAir sensors) and examined total carbon (TC) and its organic carbon (OC) and elemental carbon (EC) fractions in total suspended particles (TSP). We also investigated the dominant sources of carbonaceous aerosol using air mass backward-trajectories from the National Oceanic and Atmospheric Administration (NOAA) Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model and radiocarbon source apportionment of TC. We found TC concentrations were about twice as high in the Interior than on the coast and that modern sources were the dominant sources of carbonaceous aerosol at both Toolik (95–99%) and Utqiaġvik (86–89%), with minor contributions from fossil sources. Periods of significantly elevated PM, TC, OC, and EC concentrations coincided with major boreal forest fire activity in North America that brought smoke to the region. The radiocarbon signature of EC measured at Toolik during these wildfire smoke events indicated that over 90% of the EC originated from modern sources. Our measurements demonstrate changing aerosol concentrations in the Arctic during the summer, and emphasize the need for continuous atmospheric monitoring to evaluate and advance our understanding of this rapidly changing atmospheric environment. (Manuscript in prep) 
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  2. 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 Utqiaġvik, 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. 
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