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

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

doi:10.1073/pnas.1919723117

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

Journal Article · Tue Feb 25 00:00:00 EST 2020 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1919723117· OSTI ID:1601526

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; 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

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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: SC0012704; SC0011935; AC05-76RL01830

OSTI ID:: 1601526

Alternate ID(s):: OSTI ID: 1603276; OSTI ID: 1607676

Report Number(s):: BNL-213663-2020-JAAM; PNNL-SA-151749

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Vol. 117 Journal Issue: 10; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 65 works

Citation information provided by
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