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

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 particlemore » surface tension and viscosity, and contribute to tarball formation during aging in BB smoke. Finally, 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.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2];  [3];  [4];  [4];  [4]; ORCiD logo [5];  [1];  [6];  [7];  [8]
  1. Meteorological Research Inst., Tsukuba (Japan). Dept. of Atmosphere, Ocean and Earth System Modeling Research
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States); Washington Univ., St. Louis, MO (United States)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  5. Aerodyne Research Inc., Billerica, MA (United States). Center for Sensor Systems and Technology
  6. National Inst. for Environmental Studies, Tsukuba (Japan)
  7. Univ. of Tokyo (Japan)
  8. Arizona State Univ., Tempe, AZ (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1564418
Alternate Identifier(s):
OSTI ID: 1559998; OSTI ID: 1570765
Report Number(s):
BNL-212046-2019-JAAM; PNNL-SA-140926
Journal ID: ISSN 0027-8424
Grant/Contract Number:  
SC0012704; KP1701000/57131; SC0014287; AC06-76RLO1830; 20568; AC05-76RL01830
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 09 BIOMASS FUELS; transmission electron microscopy; organic aerosol; climate change; biomass burning; tarball

Citation Formats

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, and Buseck, Peter R. Spherical tarball particles form through rapid chemical and physical changes of organic matter in biomass-burning smoke. United States: N. p., 2019. Web. doi: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. United States. doi: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, and Buseck, Peter R. Thu . "Spherical tarball particles form through rapid chemical and physical changes of organic matter in biomass-burning smoke". United States. doi:10.1073/pnas.1900129116.
@article{osti_1564418,
title = {Spherical tarball particles form through rapid chemical and physical changes of organic matter in biomass-burning smoke},
author = {Adachi, Kouji and Sedlacek, Arthur J. and Kleinman, Lawrence and Springston, Stephen R. and Wang, Jian and Chand, Duli and Hubbe, John M. and Shilling, John E. and Onasch, Timothy B. and Kinase, Takeshi and Sakata, Kohei and Takahashi, Yoshio and Buseck, Peter R.},
abstractNote = {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. Finally, 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.},
doi = {10.1073/pnas.1900129116},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = ,
volume = ,
place = {United States},
year = {2019},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1073/pnas.1900129116

Figures / Tables:

Figure 1 Figure 1: Changes of (a) tarball number fractions, (b) non-sulfate N/K within non-tarball particles, and (c) non-sulfate O/K within non-tarball particles as photochemical ages increase for each flight. Error bars indicate the 95% confidence intervals. Numbers of measured non-tarball particles for the EDS analyses are 2451, 3271, 1962, and 2085more » for Flight#1, 2, 3, and 4, respectively. Averaged values of non-sulfate N/K of tarballs are 6.7±0.1, 2.9±0.3, 2.2±0.2, and 0.9±0.2 and those of O/K are 47.6±0.1, 14.1±0.3, 9.9±0.2, and 10.4±0.3 for flight#1, 2, 3, and 4. All ratios are calculated from weight percents.« less

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