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Creators/Authors contains: "Reeves, J. Michael"

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  1. Iodine is an atmospheric trace element emitted from oceans that efficiently destroys ozone (O 3 ). Low O 3 in airborne dust layers is frequently observed but poorly understood. We show that dust is a source of gas-phase iodine, indicated by aircraft observations of iodine monoxide (IO) radicals inside lofted dust layers from the Atacama and Sechura Deserts that are up to a factor of 10 enhanced over background. Gas-phase iodine photochemistry, commensurate with observed IO, is needed to explain the low O 3 inside these dust layers (below 15 ppbv; up to 75% depleted). The added dust iodine can explain decreases in O 3 of 8% regionally and affects surface air quality. Our data suggest that iodate reduction to form volatile iodine species is a missing process in the geochemical iodine cycle and presents an unrecognized aeolian source of iodine. Atmospheric iodine has tripled since 1950 and affects ozone layer recovery and particle formation. 
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  2. Abstract Small cumulus clouds over the western United States were measured via airborne instruments during the wildfire season in summer of 2018. Statistics of the sampled clouds are presented and compared to smoke aerosol properties. Cloud droplet concentrations were enhanced in regions impacted by biomass burning smoke, at times exceeding 3,000 cm−3. Images and elemental composition of individual smoke particles and cloud droplet residuals are presented and show that most are dominantly organic, internally mixed with some inorganic elements. Despite their high organic content and relatively low hygroscopicity, on average about half of smoke aerosol particles >80 nm diameter formed cloud droplets. This reduced cloud droplet size in small, smoke‐impacted clouds. A number of complex and competing climatic impacts may result from wide‐spread reductions in cloud droplet size due to wildfires prevalent across the region during summer months. 
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  3. Abstract We use observations from the 2015 Wintertime Investigation of Transport, Emissions, and Reactivity (WINTER) aircraft campaign to constrain the proposed mechanism of Cl2production from ClNO2reaction in acidic particles. To reproduce Cl2concentrations observed during WINTER with a chemical box model that includes ClNO2reactive uptake to form Cl2, the model required the ClNO2reaction probability, γ (ClNO2), to range from 6 × 10−6to 7 × 10−5, with a mean value of 2.3 × 10−5(±1.8 × 10−5). These field‐determined γ (ClNO2) are more than an order of magnitude lower than those determined in previous laboratory experiments on acidic surfaces, even when calculated particle pH is ≤2. We hypothesize this is because thick salt films in the laboratory enhanced the reactive uptake ClNO2compared to that which would occur in submicron aerosol particles. Using the reacto‐diffusive length‐scale framework, we show that the field and laboratory observations can be reconciled if the net aqueous‐phase reaction rate constant for ClNO2(aq) + Cl(aq) in acidic particles is on the order of 104s−1. We show that wet particle diameter and particulate chloride mass together explain 90% of the observed variance in the box model‐derived γ (ClNO2), implying that the availability of chloride and particle volume limit the efficiency of the reaction. Despite a much lower conversion of ClNO2into Cl2, this mechanism can still be responsible for the nocturnal formation of 10–20 pptv of Cl2in polluted regions, yielding an atmospherically relevant concentration of Cl atoms the following morning. 
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