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  1. Isoprene emitted by vegetation is an important precursor of secondary organic aerosol (SOA), but the mechanism and yields are uncertain. Aerosol is prevailingly aqueous under the humid conditions typical of isoprene-emitting regions. Here we develop an aqueous-phase mechanism for isoprene SOA formation coupled to a detailed gas-phase isoprene oxidation scheme. The mechanism is based on aerosol reactive uptake coefficients (γ) for water-soluble isoprene oxidation products, including sensitivity to aerosol acidity and nucleophile concentrations. We apply this mechanism to simulation of aircraft (SEAC4RS) and ground-based (SOAS) observations over the southeast US in summer 2013 using the GEOS-Chem chemical transport model. Emissions of nitrogen oxides (NOx  ≡  NO + NO2) over the southeast US are such that the peroxy radicals produced from isoprene oxidation (ISOPO2) react significantly with both NO (high-NOx pathway) and HO2 (low-NOx pathway), leading to different suites of isoprene SOA precursors. We find a mean SOA mass yield of 3.3 % from isoprene oxidation, consistent with the observed relationship of total fine organic aerosol (OA) and formaldehyde (a product of isoprene oxidation). Isoprene SOA production is mainly contributed by two immediate gas-phase precursors, isoprene epoxydiols (IEPOX, 58 % of isoprene SOA) from the low-NOx pathway and glyoxal (28 %) from both low- and high-NOx pathways. This speciation is consistent with observations of IEPOX SOA from SOAS and SEAC4RS. Observations show a strong relationship between IEPOX SOA and sulfate aerosol that we explain as due to the effect of sulfate on aerosol acidity and volume. Isoprene SOA concentrations increase as NOx emissions decrease (favoring the low-NOx pathway for isoprene oxidation), but decrease more strongly as SO2 emissions decrease (due to the effect of sulfate on aerosol acidity and volume). The US Environmental Protection Agency (EPA) projects 2013–2025 decreases in anthropogenic emissions of 34 % for NOx (leading to a 7 % increase in isoprene SOA) and 48 % for SO2 (35 % decrease in isoprene SOA). Reducing SO2 emissions decreases sulfate and isoprene SOA by a similar magnitude, representing a factor of 2 co-benefit for PM2.5 from SO2 emission controls. 
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  2. Abstract

    The convectively driven transport of soluble trace gases from the lower to the upper troposphere can occur on timescales of less than an hour, and recent studies suggest that microphysical scavenging is the dominant removal process of tropospheric ozone precursors. We examine the processes responsible for vertical transport, entrainment, and scavenging of soluble ozone precursors (formaldehyde and peroxides) for midlatitude convective storms sampled on 2 September 2013 during the Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) study. Cloud‐resolving simulations using the Weather Research and Forecasting with Chemistry model combined with aircraft measurements were performed to understand the effect of entrainment, scavenging efficiency (SE), and ice physics processes on these trace gases. Analysis of the observations revealed that the SEs of formaldehyde (43–53%) and hydrogen peroxide (~80–90%) were consistent between SEAC4RS storms and the severe convection observed during the Deep Convective Clouds and Chemistry Experiment (DC3) campaign. However, methyl hydrogen peroxide SE was generally smaller in the SEAC4RS storms (4%–27%) compared to DC3 convection. Predicted ice retention factors exhibit different values for some species compared to DC3, and we attribute these differences to variations in net precipitation production. The analyses show that much larger production of precipitation between condensation and freezing levels for DC3 severe convection compared to smaller SEAC4RS storms is largely responsible for the lower amount of soluble gases transported to colder temperatures, reducing the amount of soluble gases which eventually interact with cloud ice particles.

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