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  1. Abstract

    Organic nitrates (RONO2) are an important NOxsink. In warm, rural environments dominated by biogenic emissions, nocturnal NO3‐initiated production of RONO2is competitive with daytime OH‐initiated RONO2production. However, in urban areas, OH‐initiated production of RONO2has been assumed dominant and NO3‐initiated production considered negligible. We show evidence for nighttime RONO2production similar in magnitude to daytime production during three aircraft campaigns in chemically distinct summertime environments: Studies of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS) in the rural Southeastern United States, Front Range Air Pollution and Photochemistry Experiment (FRAPPÉ) in the Colorado Front Range, and Korea‐United States Air Quality Study (KORUS‐AQ) around the megacity of Seoul. During each campaign, morning observations show RONO2enhancements at constant, near‐background Ox(≡ O3+NO2) concentrations, indicating that the RONO2are from a non‐photochemical source, whereas afternoon observations show a strong correlation between RONO2and Oxresulting from photochemical production. We show that there are sufficient precursors for nighttime RONO2formation during all three campaigns. This evidence impacts our understanding of nighttime NOxchemistry.

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  2. Abstract

    We analyze the effects of the diurnal cycle of fire emissions (DCFE) and plume rise on U.S. air quality using the MUSICAv0 (Multi‐Scale Infrastructure for Chemistry and Aerosols Version 0) model during the FIREX‐AQ (Fire Influence on Regional to Global Environments and Air Quality) and WE‐CAN (Western wildfire Experiment for Cloud chemistry, Aerosol absorption and Nitrogen) field campaigns. To include DCFE in the model, we employ two approaches: a DCFE climatology and DCFE derived from a satellite fire radiative power product. We also implemented two sets of plume‐rise climatologies, and two plume‐rise parameterizations. We evaluate the model performance with airborne measurements, U.S. EPA Air Quality System surface measurements, and satellite products. Overall, including plume rise improves model agreement with observations such as aircraft observations of CO and NOxfor FIREX‐AQ and WE‐CAN. Applying DCFE also improves model performance, such as for surface PM2.5in fire‐impacted regions. The impact of plume rise is larger than the impact of DCFE. Plume rise can greatly enhance modeled long‐range transport of fire‐emitted pollutants. The simulations with plume‐rise parameterizations generally perform better than the simulations with plume‐rise climatologies during FIREX‐AQ, but not for WE‐CAN. The 2019 Williams Flats Fire case study demonstrates that DCFE and plume rise change fire impacts because fire emissions are subject to different meteorology and chemistry when emitted at different times of a day and altitudes. Moreover, DCFE and plume rise also impact local‐to‐regional meteorology and chemical reaction rates. DCFE and plume rise will be included in future MUSICA versions.

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  3. Abstract

    Reactive nitrogen (Nr) within smoke plumes plays important roles in the production of ozone, the formation of secondary aerosols, and deposition of fixed N to ecosystems. The Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen (WE‐CAN) field campaign sampled smoke from 23 wildfires throughout the western U.S. during summer 2018 using the NSF/NCAR C‐130 research aircraft. We empirically estimateNrnormalized excess mixing ratios and emission factors from fires sampled within 80 min of estimated emission and explore variability in the dominant forms ofNrbetween these fires. We find that reduced N compounds comprise a majority (39%–80%; median = 66%) of total measured reactive nitrogen (ΣNr) emissions. The smoke plumes sampled during WE‐CAN feature rapid chemical transformations after emission. As a result, within minutes after emission total measured oxidized nitrogen (ΣNOy) and measured totalΣNHx(NH3 + pNH4) are more robustly correlated with modified combustion efficiency (MCE) than NOxand NH3by themselves. The ratio of ΣNHx/ΣNOydisplays a negative relationship with MCE, consistent with previous studies. A positive relationship with total measuredΣNrsuggests that both burn conditions and fuel N content/volatilization differences contribute to the observed variability in the distribution of reduced and oxidizedNr. Additionally, we compare our in situ field estimates ofNrEFs to previous lab and field studies. For similar fuel types, we findΣNHxEFs are of the same magnitude or larger than lab‐based NH3EF estimates, andΣNOyEFs are smaller than lab NOxEFs.

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  4. Abstract

    Wildfires are a major source of gas‐phase ammonia (NH3) to the atmosphere. Quantifying the evolution and fate of this NH3is important to understanding the formation of secondary aerosol in smoke and its accompanying effects on radiative balance and nitrogen deposition. Here, we use data from the Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen (WE‐CAN) to add new empirical constraints on the e‐folding loss timescale of NH3and its relationship with particulate ammonium (pNH4) within wildfire smoke plumes in the western U.S. during summer 2018. We show that the e‐folding loss timescale of NH3with respect to particle‐phase partitioning ranges from ∼24 to ∼4000 min (median of 55 min). Within these same plumes, oxidation of nitrogen oxides is observed concurrent with increases in the fraction ofpNH4in each plume sampled, suggesting that formation of ammonium nitrate (NH4NO3) is likely. We find wide variability in how close ourin situmeasurements of NH4NO3are to those expected in a dry thermodynamic equilibrium, and find that NH4NO3is most likely to form in fresh, dense smoke plumes injected at higher altitudes and colder temperatures. In chemically older smoke we observe correlations between both the fraction ofpNH4and the fraction of particulate nitrate (pNO3) in the aerosol with temperature, providing additional evidence of the presence of NH4NO3and the influence of injection height on gas‐particle partitioning of NH3.

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  5. Abstract

    We present a comparison of instruments measuring nitrogen oxide species from an aircraft during the 2015 Wintertime INvestigation of Transport, Emissions, and Reactivity (WINTER) campaign over the northeast United States. Instrument techniques compared here include chemiluminescence (CL), thermal dissociation laser‐induced fluorescence (TD‐LIF), cavity ring‐down spectroscopy (CRDS), high‐resolution time of flight, iodide‐adduct chemical ionization mass spectrometry (ICIMS), and aerosol mass spectrometry. Species investigated include NO2, NO, total nitrogen oxides (NOy), N2O5, ClNO2, and HNO3. Particulate‐phase nitrate is also included for comparisons of HNO3and NOy. Instruments generally agreed within reported uncertainties, with individual flights sometimes showing much better agreement than the data set taken as a whole, due to flight‐to‐flight slope changes. NO measured by CRDS and CL showed an average relative slope of 1.16 ± 0.01 across all flights, which is outside of combined uncertainties. The source of the error was not identified. For NO2measured by CRDS and TD‐LIF the average was 1.02 ± 0.00; for NOymeasured by CRDS and CL the average was 1.01 ± 0.00; and for N2O5measured by CRDS and ICIMS the average was 0.89 ± 0.01. NOybudget closure to within 20% is demonstrated. We observe nonlinearity in NO2and NOycorrelations at concentrations above ~30 ppbv that may be related to the NO discrepancy noted above. For ClNO2there were significant differences between ICIMS and TD‐LIF, potentially due in part to the temperature used for thermal dissociation. Although the fraction of particulate nitrate measured by the TD‐LIF is not well characterized, it improves comparisons to include particulate measurements.

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  6. Abstract

    Sulfur dioxide (SO2) is emitted in large quantities from coal‐burning power plants and leads to various harmful health and environmental effects. In this study, we use plume intercepts from the Wintertime INvestigation of Transport, Emission and Reactivity (WINTER) campaign to estimate the oxidation rates of SO2under wintertime conditions and the factors that determine SO2removal. Observations suggest that OH governs the rate SO2oxidation in the eastern United States during winter. The range of mean oxidation rates during the day from power plants were 0.22–0.71%/hr, producing SO2lifetimes of 13–43 days, if SO2consumption is assumed to occur during 10.5 hr of daylight in cloudless conditions. Though most nighttime rate measurements were zero within uncertainty, there is some evidence of nighttime removal, which suggests alternate oxidation mechanisms. The fastest nighttime observed SO2oxidation rate was 0.25±0.07%/hr, producing a combined day/night SO2lifetime of 8.5–21 days. The upper limit of the oxidation rate (the mean+1σof the fastest day and night observations) is 16.5%/day, corresponding to a lifetime of 6.1 days. The analysis also quantifies the primary emission of sulfate from power plants. The median mole percentage of SO4‐2from observed plumes was 1.7% and the mean percentage sulfate was 2.8% for intercepts within 1 hr of transit to power plants. The largest value observed from close intercepts was over 7% sulfate, and the largest extrapolated value was 18%, based on intercepts further from their source and fastest observed oxidation rate.

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