Chemical Imaging of Atmospheric Biomass Burning Particles from North American Wildfires

Rivera-Adorno, Felipe A.; Tomlin, Jay M.; Lata, Nurun Nahar; Azzarello, Lisa; Robinson, Michael A.; Washenfelder, Rebecca A.; Franchin, Alessandro; Middlebrook, Ann M.; China, Swarup; Brown, Steven S.; Young, Cora J.; Fraund, Matthew; Moffet, Ryan C.; Laskin, Alexander

doi:10.1021/acsestair.4c00242

Chemical Imaging of Atmospheric Biomass Burning Particles from North American Wildfires

Journal Article · Tue Apr 01 00:00:00 EDT 2025 · ACS ES&T Air

DOI:https://doi.org/10.1021/acsestair.4c00242· OSTI ID:2555800

^[1]; ^[1]; ^[2]; ^[3]; Robinson, Michael A. ^[4]; ^[5]; Franchin, Alessandro ^[6]; ^[5]; ^[2]; ^[4]; ^[3]; ^[7]; ^[8]; ^[1]

Purdue University, West Lafayette, IN (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
York University, Toronto, ON (Canada)
National Oceanic and Atmospheric Administration, Boulder, CO (United States); University of Colorado, Boulder, CO (United States)
National Oceanic and Atmospheric Administration, Boulder, CO (United States)
University Corporation for Atmospheric Research, Boulder, CO (United States)
Fraund Consulting, Pleasant Hill, CA (United States)
Sonoma Technology, Inc., Petaluma, CA (United States)

The effects of biomass burning aerosols (BBA) on radiative forcing and cloud formation depend on chemical composition and the internal structures of individual particles within smoke plumes. To improve our understanding of the chemical and physical properties of BBA emitted at different times of the day and their evolution during atmospheric aging, we conducted a study as a part of the Fire Influence on Regional to Global Environments and Air Quality field campaign. Particle samples were collected onboard a research aircraft from smoke plumes from a wildfire in eastern Oregon during late afternoon and nighttime flights on August 28, 2019. A time-resolved aerosol collector was used to collect samples on substrates for offline spectromicroscopic imaging to investigate the single-particle characteristics of BBA particles. Approximately 20,400 individual particles from 10 selected samples were analyzed using computer-controlled scanning electron microscopy coupled with energy-dispersive X-ray microanalysis, revealing their elemental composition, morphology, and viscosity. Elemental microanalysis indicated that aged potassium is likely found in the form of K₂SO₄, KNO₃, and possible K-organic salts. Further chemical speciation and carbon bonding mapping within individual particles were conducted using synchrotron-based scanning transmission X-ray microscopy (STXM) coupled with near edge X-ray absorption fine structure (NEXAFS) spectroscopy. Real-time, water-soluble light absorption measurements were acquired using a particle-into-liquid sampler instrument coupled to a liquid waveguide capillary cell and total organic analyzer. In the late afternoon samples, 65% of the total particle number population consisted entirely of organic components, compared to 46% in the nighttime particles. These differences were attributed to discrepancies in composition at the time of emission and to the daytime condensation and accumulation of photochemically formed secondary organic material on existing BBA particles, a process that halts at night. Microscopy images indicated that particle viscosity was lower in the nighttime particles (<10¹ Pa·s), likely due to increased relative humidity and a higher contribution from hygroscopic inorganic components. The chemical heterogeneity of individual particles was quantified using STXM-derived mixing state parameters. The nature of carbon bonding within individual particles was inferred from the extent of carbon sp² hybridization derived from NEXAFS spectra. Average percentages of sp² hybridization range between 40% and 60%, with no noticeable differences between late afternoon and nighttime flights. These findings were compared with the online optical properties of both late afternoon and nighttime smoke plumes, providing valuable insights into the complex relationship between chemical composition and optical properties of BBA particles at different times of the day.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Purdue University, West Lafayette, IN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: SC0021977

OSTI ID:: 2555800

Alternate ID(s):: OSTI ID: 2574390

Report Number(s):: PNNL-SA--205265

Journal Information:: ACS ES&T Air, Journal Name: ACS ES&T Air Journal Issue: 4 Vol. 2; ISSN 2837-1402

Publisher:: ACS PublicationsCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
54 ENVIRONMENTAL SCIENCES
X-ray microscopy
aerosols
atmopsheric science
atmospheric particles
biomass burning emissions
chemical imaging
electron microscopy
particle mixing state
particles
particulate matter
redox reactions

Chemical Imaging of Atmospheric Biomass Burning Particles from North American Wildfires

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