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Title: Radiative absorption enhancements by black carbon controlled by particle-to-particle heterogeneity in composition

Abstract

Black carbon (BC) absorbs solar radiation, leading to a strong but uncertain warming effect on climate. A key challenge in modeling and quantifying BC’s radiative effect on climate is predicting enhancements in light absorption that result from internal mixing between BC and other aerosol components. Modeling and laboratory studies show that BC, when mixed with other aerosol components, absorbs more strongly than pure, uncoated BC; however, some ambient observations suggest more variable and weaker absorption enhancement. We show that the lower-than-expected enhancements in ambient measurements result from a combination of two factors. First, the often used spherical, concentric core-shell approximation generally overestimates the absorption by BC. Second, and more importantly, inadequate consideration of heterogeneity in particle-to-particle composition engenders substantial overestimation in absorption by the total particle population, with greater heterogeneity associated with larger model–measurement differences. We show that accounting for these two effects—variability in per-particle composition and deviations from the core-shell approximation—reconciles absorption enhancement predictions with laboratory and field observations and resolves the apparent discrepancy. Furthermore, our consistent model framework provides a path forward for improving predictions of BC’s radiative effect on climate.

Authors:
ORCiD logo; ORCiD logo; ; ; ; ; ; ; ; ; ; ;
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:
1601526
Alternate Identifier(s):
OSTI ID: 1603276; OSTI ID: 1607676
Report Number(s):
[BNL-213663-2020-JAAM; PNNL-SA-151749]
[Journal ID: ISSN 0027-8424; /pnas/117/10/5196.atom]
Grant/Contract Number:  
[SC0012704; SC0011935; 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 Volume: 117 Journal Issue: 10]; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; black carbon; direct radiative forcing; absorption enhancement; aerosol mixing state

Citation Formats

Fierce, Laura, Onasch, Timothy B., Cappa, Christopher D., Mazzoleni, Claudio, China, Swarup, Bhandari, Janarjan, Davidovits, Paul, Fischer, D. Al, Helgestad, Taylor, Lambe, Andrew T., Sedlacek, III, Arthur J., Smith, Geoffrey D., and Wolff, Lindsay. Radiative absorption enhancements by black carbon controlled by particle-to-particle heterogeneity in composition. United States: N. p., 2020. Web. doi:10.1073/pnas.1919723117.
Fierce, Laura, Onasch, Timothy B., Cappa, Christopher D., Mazzoleni, Claudio, China, Swarup, Bhandari, Janarjan, Davidovits, Paul, Fischer, D. Al, Helgestad, Taylor, Lambe, Andrew T., Sedlacek, III, Arthur J., Smith, Geoffrey D., & Wolff, Lindsay. Radiative absorption enhancements by black carbon controlled by particle-to-particle heterogeneity in composition. United States. doi:10.1073/pnas.1919723117.
Fierce, Laura, Onasch, Timothy B., Cappa, Christopher D., Mazzoleni, Claudio, China, Swarup, Bhandari, Janarjan, Davidovits, Paul, Fischer, D. Al, Helgestad, Taylor, Lambe, Andrew T., Sedlacek, III, Arthur J., Smith, Geoffrey D., and Wolff, Lindsay. Tue . "Radiative absorption enhancements by black carbon controlled by particle-to-particle heterogeneity in composition". United States. doi:10.1073/pnas.1919723117.
@article{osti_1601526,
title = {Radiative absorption enhancements by black carbon controlled by particle-to-particle heterogeneity in composition},
author = {Fierce, Laura and Onasch, Timothy B. and Cappa, Christopher D. and Mazzoleni, Claudio and China, Swarup and Bhandari, Janarjan and Davidovits, Paul and Fischer, D. Al and Helgestad, Taylor and Lambe, Andrew T. and Sedlacek, III, Arthur J. and Smith, Geoffrey D. and Wolff, Lindsay},
abstractNote = {Black carbon (BC) absorbs solar radiation, leading to a strong but uncertain warming effect on climate. A key challenge in modeling and quantifying BC’s radiative effect on climate is predicting enhancements in light absorption that result from internal mixing between BC and other aerosol components. Modeling and laboratory studies show that BC, when mixed with other aerosol components, absorbs more strongly than pure, uncoated BC; however, some ambient observations suggest more variable and weaker absorption enhancement. We show that the lower-than-expected enhancements in ambient measurements result from a combination of two factors. First, the often used spherical, concentric core-shell approximation generally overestimates the absorption by BC. Second, and more importantly, inadequate consideration of heterogeneity in particle-to-particle composition engenders substantial overestimation in absorption by the total particle population, with greater heterogeneity associated with larger model–measurement differences. We show that accounting for these two effects—variability in per-particle composition and deviations from the core-shell approximation—reconciles absorption enhancement predictions with laboratory and field observations and resolves the apparent discrepancy. Furthermore, our consistent model framework provides a path forward for improving predictions of BC’s radiative effect on climate.},
doi = {10.1073/pnas.1919723117},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = [10],
volume = [117],
place = {United States},
year = {2020},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
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DOI: 10.1073/pnas.1919723117

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