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 language | English (US) |
|---|---|
| Pages (from-to) | 19336-19341 |
| Number of pages | 6 |
| Journal | Proceedings of the National Academy of Sciences of the United States of America |
| Volume | 116 |
| Issue number | 39 |
| DOIs | |
| State | Published - Sep 24 2019 |
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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 journal › Article
}
TY - JOUR
T1 - Spherical tarball particles form through rapid chemical and physical changes of organic matter in biomass-burning smoke
AU - Adachi, Kouji
AU - Sedlacek, Arthur J.
AU - Kleinman, Lawrence
AU - Springston, Stephen R.
AU - Wang, Jian
AU - Chand, Duli
AU - Hubbe, John M.
AU - Shilling, John E.
AU - Onasch, Timothy B.
AU - Kinase, Takeshi
AU - Sakata, Kohei
AU - Takahashi, Yoshio
AU - Buseck, Peter R.
PY - 2019/9/24
Y1 - 2019/9/24
N2 - 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.
AB - 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.
KW - Biomass burning
KW - Climate change
KW - Organic aerosol
KW - Tarball
KW - Transmission electron microscopy
UR - http://www.scopus.com/inward/record.url?scp=85072642515&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85072642515&partnerID=8YFLogxK
U2 - 10.1073/pnas.1900129116
DO - 10.1073/pnas.1900129116
M3 - Article
C2 - 31488715
AN - SCOPUS:85072642515
VL - 116
SP - 19336
EP - 19341
JO - Proceedings of the National Academy of Sciences of the United States of America
JF - Proceedings of the National Academy of Sciences of the United States of America
SN - 0027-8424
IS - 39
ER -