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Abstract Wildfire emissions affect downwind air quality and human health. Predictions of these impacts using models are limited by uncertainties in emissions and chemical evolution of smoke plumes. Using high‐time‐resolution aircraft measurements, we illustrate spatial variations that can exist within a plume due to differences in the photochemical environment. Horizontal and vertical crosswind gradients of dilution‐corrected mixing ratios were observed in midday plumes for reactive compounds and their oxidation products, such as nitrous acid, catechol, and ozone, likely due to faster photochemistry in optically thinner plume edges relative to darker plume cores. Gradients in plumes emitted close to sunset are characterized by titration of O3in the plume and reduced or no gradient formation. We show how crosswind gradients can lead to underestimated emission ratios for reactive compounds and overestimated emission ratios for oxidation products. These observations will lead to improved predictions of wildfire emissions, evolution, and impacts across daytime and nighttime.
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Reactive Nitrogen Partitioning Enhances the Contribution of Canadian Wildfire Plumes to US Ozone Air Quality
Quantifying the variable impacts of wildfire smoke on ozone air quality is challenging. Here we use airborne measurements from the 2018 Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen (WE-CAN) to parameterize emissions of reactive nitrogen (NOy) from wildfires into peroxyacetyl nitrate (PAN; 37%), NO3− (27%), and NO (36%) in a global chemistry-climate model with 13 km spatial resolution over the contiguous US. The NOy partitioning, compared with emitting all NOy as NO, reduces model ozone bias in near-fire smoke plumes sampled by the aircraft and enhances ozone downwind by 5–10 ppbv when Canadian smoke plumes travel to Washington, Utah, Colorado, and Texas. Using multi-platform observations, we identify the smoke-influenced days with daily maximum 8-hr average (MDA8) ozone of 70–88 ppbv in Kennewick, Salt Lake City, Denver and Dallas. On these days, wildfire smoke enhanced MDA8 ozone by 5–25 ppbv, through ozone produced remotely during plume transport and locally via interactions of smoke plume with urban emissions.
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- PAR ID:
- 10572485
- Publisher / Repository:
- Wiley
- Date Published:
- Journal Name:
- Geophysical Research Letters
- Volume:
- 51
- Issue:
- 15
- ISSN:
- 0094-8276
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1029/2024GL109369
