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. 2021 Dec 7;55(23):15646-15657.
doi: 10.1021/acs.est.1c03803. Epub 2021 Nov 24.

Novel Analysis to Quantify Plume Crosswind Heterogeneity Applied to Biomass Burning Smoke

Zachary C J Decker  1   2   3 , Siyuan Wang  1   2 , Ilann Bourgeois  1   2 , Pedro Campuzano Jost  2   3 , Matthew M Coggon  1   2 , Joshua P DiGangi  4 , Glenn S Diskin  4 , Frank M Flocke  5 , Alessandro Franchin  1   2   5 , Carley D Fredrickson  6 , Georgios I Gkatzelis  1   2 , Samuel R Hall  5 , Hannah Halliday  5 , Katherine Hayden  7 , Christopher D Holmes  8 , L Gregory Huey  9 , Jose L Jimenez  2   3 , Young Ro Lee  9 , Jakob Lindaas  10 , Ann M Middlebrook  1 , Denise D Montzka  5 , J Andrew Neuman  1   2 , John B Nowak  11 , Demetrios Pagonis  2   3 , Brett B Palm  6 , Jeff Peischl  1   2 , Felix Piel  12   13 , Pamela S Rickly  1   2 , Michael A Robinson  1   2   3 , Andrew W Rollins  1 , Thomas B Ryerson  1 , Kanako Sekimoto  14 , Joel A Thornton  6 , Geoff S Tyndall  5 , Kirk Ullmann  5 , Patrick R Veres  1 , Carsten Warneke  1   2 , Rebecca A Washenfelder  1 , Andrew J Weinheimer  5 , Armin Wisthaler  12   13 , Caroline Womack  1   2 , Steven S Brown  1   3
Affiliations

Novel Analysis to Quantify Plume Crosswind Heterogeneity Applied to Biomass Burning Smoke

Zachary C J Decker et al. Environ Sci Technol. .

Abstract

We present a novel method, the Gaussian observational model for edge to center heterogeneity (GOMECH), to quantify the horizontal chemical structure of plumes. GOMECH fits observations of short-lived emissions or products against a long-lived tracer (e.g., CO) to provide relative metrics for the plume width (wi/wCO) and center (bi/wCO). To validate GOMECH, we investigate OH and NO3 oxidation processes in smoke plumes sampled during FIREX-AQ (Fire Influence on Regional to Global Environments and Air Quality, a 2019 wildfire smoke study). An analysis of 430 crosswind transects demonstrates that nitrous acid (HONO), a primary source of OH, is narrower than CO (wHONO/wCO = 0.73-0.84 ± 0.01) and maleic anhydride (an OH oxidation product) is enhanced on plume edges (wmaleicanhydride/wCO = 1.06-1.12 ± 0.01). By contrast, NO3 production [P(NO3)] occurs mainly at the plume center (wP(NO3)/wCO = 0.91-1.00 ± 0.01). Phenolic emissions, highly reactive to OH and NO3, are narrower than CO (wphenol/wCO = 0.96 ± 0.03, wcatechol/wCO = 0.91 ± 0.01, and wmethylcatechol/wCO = 0.84 ± 0.01), suggesting that plume edge phenolic losses are the greatest. Yet, nitrophenolic aerosol, their oxidation product, is the greatest at the plume center (wnitrophenolicaerosol/wCO = 0.95 ± 0.02). In a large plume case study, GOMECH suggests that nitrocatechol aerosol is most associated with P(NO3). Last, we corroborate GOMECH with a large eddy simulation model which suggests most (55%) of nitrocatechol is produced through NO3 in our case study.

Keywords: FIREX-AQ; HONO; LES model; biomass burning; catechol; phenolics; plume shape; wildfire.

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