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Title: Quantification of black carbon mixing state from traffic: Implications for aerosol optical properties

Abstract

The climatic impacts of black carbon (BC) aerosol, an important absorber of solar radiation in the atmosphere, remain poorly constrained and are intimately related to its particle-scale physical and chemical properties. Using particle-resolved modelling informed by quantitative measurements from a soot-particle aerosol mass spectrometer, we confirm that the mixing state (the distribution of co-emitted aerosol amongst fresh BC-containing particles) at the time of emission significantly affects BC-aerosol optical properties even after a day of atmospheric processing. Both single particle and ensemble aerosol mass spectrometry observations indicate that BC near the point of emission co-exists with hydrocarbon-like organic aerosol (HOA) in two distinct particle types: HOA-rich and BC-rich particles. The average mass fraction of black carbon in HOA-rich and BC-rich particle classes was < 0.1 and 0.8, respectively. Notably, approximately 90 % of BC mass resides in BC-rich particles. This new measurement capability provides quantitative insight into the physical and chemical nature of BC-containing particles and is used to drive a particle-resolved aerosol box model. Lastly, significant differences in calculated single scattering albedo (an increase of 0.1) arise from accurate treatment of initial particle mixing state as compared to the assumption of uniform aerosol composition at the point of BC injectionmore » into the atmosphere.« less

Authors:
 [1];  [2];  [3];  [3];  [1];  [1];  [4];  [1];  [5];  [1]
  1. Univ. of Toronto, Toronto, ON (Canada)
  2. Univ. of Toronto, Toronto, ON (Canada); Univ. College Cork, Cork (Ireland)
  3. Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States)
  4. Univ. College Cork, Cork (Ireland)
  5. University of Toronto, Toronto, Ontario, (Canada). Department of Chemistry
Publication Date:
Research Org.:
Univ. of Illinois at Urbana-Champaign, IL (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1258010
Grant/Contract Number:  
SC0011771
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 16; Journal Issue: 7; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Willis, Megan D., Healy, Robert M., Riemer, Nicole, West, Matthew, Wang, Jon M., Jeong, Cheol -Heon, Wenger, John C., Evans, Greg J., Abbatt, Jonathan P. D., and Lee, Alex K. Y. Quantification of black carbon mixing state from traffic: Implications for aerosol optical properties. United States: N. p., 2016. Web. doi:10.5194/acp-16-4693-2016.
Willis, Megan D., Healy, Robert M., Riemer, Nicole, West, Matthew, Wang, Jon M., Jeong, Cheol -Heon, Wenger, John C., Evans, Greg J., Abbatt, Jonathan P. D., & Lee, Alex K. Y. Quantification of black carbon mixing state from traffic: Implications for aerosol optical properties. United States. doi:10.5194/acp-16-4693-2016.
Willis, Megan D., Healy, Robert M., Riemer, Nicole, West, Matthew, Wang, Jon M., Jeong, Cheol -Heon, Wenger, John C., Evans, Greg J., Abbatt, Jonathan P. D., and Lee, Alex K. Y. Thu . "Quantification of black carbon mixing state from traffic: Implications for aerosol optical properties". United States. doi:10.5194/acp-16-4693-2016. https://www.osti.gov/servlets/purl/1258010.
@article{osti_1258010,
title = {Quantification of black carbon mixing state from traffic: Implications for aerosol optical properties},
author = {Willis, Megan D. and Healy, Robert M. and Riemer, Nicole and West, Matthew and Wang, Jon M. and Jeong, Cheol -Heon and Wenger, John C. and Evans, Greg J. and Abbatt, Jonathan P. D. and Lee, Alex K. Y.},
abstractNote = {The climatic impacts of black carbon (BC) aerosol, an important absorber of solar radiation in the atmosphere, remain poorly constrained and are intimately related to its particle-scale physical and chemical properties. Using particle-resolved modelling informed by quantitative measurements from a soot-particle aerosol mass spectrometer, we confirm that the mixing state (the distribution of co-emitted aerosol amongst fresh BC-containing particles) at the time of emission significantly affects BC-aerosol optical properties even after a day of atmospheric processing. Both single particle and ensemble aerosol mass spectrometry observations indicate that BC near the point of emission co-exists with hydrocarbon-like organic aerosol (HOA) in two distinct particle types: HOA-rich and BC-rich particles. The average mass fraction of black carbon in HOA-rich and BC-rich particle classes was < 0.1 and 0.8, respectively. Notably, approximately 90 % of BC mass resides in BC-rich particles. This new measurement capability provides quantitative insight into the physical and chemical nature of BC-containing particles and is used to drive a particle-resolved aerosol box model. Lastly, significant differences in calculated single scattering albedo (an increase of 0.1) arise from accurate treatment of initial particle mixing state as compared to the assumption of uniform aerosol composition at the point of BC injection into the atmosphere.},
doi = {10.5194/acp-16-4693-2016},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 7,
volume = 16,
place = {United States},
year = {2016},
month = {4}
}

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