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Abstract The Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen (WE‐CAN) deployed the NSF/NCAR C‐130 aircraft in summer 2018 across the western U.S. to sample wildfire smoke during its first days of atmospheric evolution. We present a summary of a subset of reactive oxidized nitrogen species (NOy) in plumes sampled in a pseudo‐Lagrangian fashion. Emissions of nitrogen oxides (NOx = NO + NO2) and nitrous acid (HONO) are rapidly converted to more oxidized forms. Within 4 h, ∼86% of the ΣNOyis in the form of peroxy acyl nitrates (PANs) (∼37%), particulate nitrate (pNO3) (∼27%), and gas‐phase organic nitrates (Org N(g)) (∼23%). The averagee‐folding time and distance for NOxare ∼90 min and ∼40 km, respectively. Nearly no enhancements in nitric acid (HNO3) were observed in plumes sampled in a pseudo‐Lagrangian fashion, implying HNO3‐limited ammonium nitrate (NH4NO3) formation, with one notable exception that we highlight as a case study. We also summarize the observed partitioning of NOyin all the smoke samples intercepted during WE‐CAN. In smoke samples intercepted above 3 km above sea level (ASL), the contributions of PANs andpNO3to ΣNOyincrease with altitude. WE‐CAN also sampled smoke from multiple fires mixed with anthropogenic emissions over the California Central Valley. We distinguish samples where anthropogenic NOxemissions appear to lead to an increase in NOxabundances by a factor of four and contribute to additional PAN formation.
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Empirical Insights Into the Fate of Ammonia in Western U.S. Wildfire Smoke Plumes
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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- PAR ID:
- 10446055
- Author(s) / Creator(s):
- ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; more »
- Publisher / Repository:
- DOI PREFIX: 10.1029
- Date Published:
- Journal Name:
- Journal of Geophysical Research: Atmospheres
- Volume:
- 126
- Issue:
- 11
- ISSN:
- 2169-897X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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