Spherical tarball particles form through rapid chemical and physical changes of organic matter in biomass-burning smoke

Kouji Adachi, Arthur J. Sedlacek, Lawrence Kleinman, Stephen R. Springston, Jian Wang, Duli Chand, John M. Hubbe, John E. Shilling, Timothy B. Onasch, Takeshi Kinase, Kohei Sakata, Yoshio Takahashi, Peter R. Buseck

Research output: Contribution to journalArticle

1 Citation (Scopus)

Abstract

Biomass burning (BB) emits enormous amounts of aerosol particles and gases into the atmosphere and thereby significantly influences regional air quality and global climate. A dominant particle type from BB is spherical organic aerosol particles commonly referred to as tarballs. Currently, tarballs can only be identified, using microscopy, from their uniquely spherical shapes following impaction onto a grid. Despite their abundance and potential significance for climate, many unanswered questions related to their formation, emission inventory, removal processes, and optical properties still remain. Here, we report analysis that supports tarball formation in which primary organic particles undergo chemical and physical processing within ∼3 h of emission. Transmission electron microscopy analysis reveals that the number fractions of tarballs and the ratios of N and O relative to K, the latter a conserved tracer, increase with particle age and that the more-spherical particles on the substrates had higher ratios of N and O relative to K. Scanning transmission X-ray spectrometry and electron energy loss spectrometry analyses show that these chemical changes are accompanied by the formation of organic compounds that contain nitrogen and carboxylic acid. The results imply that the chemical changes increase the particle sphericity on the substrates, which correlates with particle surface tension and viscosity, and contribute to tarball formation during aging in BB smoke. These findings will enable models to better partition tarball contributions to BB radiative forcing and, in so doing, better help constrain radiative forcing models of BB events.

Original languageEnglish (US)
Pages (from-to)19336-19341
Number of pages6
JournalProceedings of the National Academy of Sciences of the United States of America
Volume116
Issue number39
DOIs
StatePublished - Sep 24 2019

Fingerprint

Smoke
Biomass
Aerosols
Climate
Optical Phenomena
Spectrum Analysis
Nitrogen Compounds
Surface Tension
Carboxylic Acids
Transmission Electron Microscopy
Atmosphere
Viscosity
Microscopy
Gases
Air
X-Rays
Electrons
Equipment and Supplies

Keywords

  • Biomass burning
  • Climate change
  • Organic aerosol
  • Tarball
  • Transmission electron microscopy

ASJC Scopus subject areas

  • General

Cite this

Spherical tarball particles form through rapid chemical and physical changes of organic matter in biomass-burning smoke. / Adachi, Kouji; Sedlacek, Arthur J.; Kleinman, Lawrence; Springston, Stephen R.; Wang, Jian; Chand, Duli; Hubbe, John M.; Shilling, John E.; Onasch, Timothy B.; Kinase, Takeshi; Sakata, Kohei; Takahashi, Yoshio; Buseck, Peter R.

In: Proceedings of the National Academy of Sciences of the United States of America, Vol. 116, No. 39, 24.09.2019, p. 19336-19341.

Research output: Contribution to journalArticle

Adachi, K, Sedlacek, AJ, Kleinman, L, Springston, SR, Wang, J, Chand, D, Hubbe, JM, Shilling, JE, Onasch, TB, Kinase, T, Sakata, K, Takahashi, Y & Buseck, PR 2019, 'Spherical tarball particles form through rapid chemical and physical changes of organic matter in biomass-burning smoke', Proceedings of the National Academy of Sciences of the United States of America, vol. 116, no. 39, pp. 19336-19341. https://doi.org/10.1073/pnas.1900129116
Adachi, Kouji ; Sedlacek, Arthur J. ; Kleinman, Lawrence ; Springston, Stephen R. ; Wang, Jian ; Chand, Duli ; Hubbe, John M. ; Shilling, John E. ; Onasch, Timothy B. ; Kinase, Takeshi ; Sakata, Kohei ; Takahashi, Yoshio ; Buseck, Peter R. / Spherical tarball particles form through rapid chemical and physical changes of organic matter in biomass-burning smoke. In: Proceedings of the National Academy of Sciences of the United States of America. 2019 ; Vol. 116, No. 39. pp. 19336-19341.
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