Condensed-phase biogenic–anthropogenic interactions with implications for cold cloud formation
Abstract
Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil-fuel combustion can acquire a coating of SOA. We investigate SOA-soot biogenic-anthropogenic interactions and their impact on ice nucleation in relation to the particles’ organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without presence of sulfate or soot particles. Corresponding particle glass transition (Tg) and full deliquescence relative humidity (FDRH) were estimated by a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfate mixtures exhibit a core-shell configuration (i.e. a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation in agreement with respective Tg and FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid inducing ice nucleation. Naphthalene SOA coated soot particles acted as IN above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not playmore »
- Authors:
-
[2];
[1]
- Stony Brook Univ., NY (United States). Inst. for Terrestrial and Planetary Atmospheres, School of Marine and Atmospheric Sciences
- Boston College, Chestnut Hill, MA (United States). Dept. of Chemistry; Aerodyne Research Inc., Billerica, MA (United States)
- Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical and Biomolecular Engineering
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Univ. of the Pacific, Stockton, CA (United States). Dept. of Chemistry
- Aerodyne Research Inc., Billerica, MA (United States)
- Univ. of California, Irvine, CA (United States). Dept. of Chemistry
- Univ. of the Pacific, Stockton, CA (United States). Dept. of Chemistry
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
- Boston College, Chestnut Hill, MA (United States). Dept. of Chemistry
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Stony Brook Univ., NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1436142
- Alternate Identifier(s):
- OSTI ID: 1349681
- Grant/Contract Number:
- AC02-05CH11231; SC0016370; SC0008613; SC0006980; SC0011935
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Faraday Discussions
- Additional Journal Information:
- Journal Volume: 200; Journal ID: ISSN 1359-6640
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES
Citation Formats
Charnawskas, Joseph C., Alpert, Peter A., Lambe, Andrew T., Berkemeier, Thomas, O' Brien, Rachel E., Massoli, Paola, Onasch, Timothy B., Shiraiwa, Manabu, Moffet, Ryan C., Gilles, Mary K., Davidovits, Paul, Worsnop, Douglas R., and Knopf, Daniel A. Condensed-phase biogenic–anthropogenic interactions with implications for cold cloud formation. United States: N. p., 2017.
Web. doi:10.1039/c7fd00010c.
Charnawskas, Joseph C., Alpert, Peter A., Lambe, Andrew T., Berkemeier, Thomas, O' Brien, Rachel E., Massoli, Paola, Onasch, Timothy B., Shiraiwa, Manabu, Moffet, Ryan C., Gilles, Mary K., Davidovits, Paul, Worsnop, Douglas R., & Knopf, Daniel A. Condensed-phase biogenic–anthropogenic interactions with implications for cold cloud formation. United States. https://doi.org/10.1039/c7fd00010c
Charnawskas, Joseph C., Alpert, Peter A., Lambe, Andrew T., Berkemeier, Thomas, O' Brien, Rachel E., Massoli, Paola, Onasch, Timothy B., Shiraiwa, Manabu, Moffet, Ryan C., Gilles, Mary K., Davidovits, Paul, Worsnop, Douglas R., and Knopf, Daniel A. Tue .
"Condensed-phase biogenic–anthropogenic interactions with implications for cold cloud formation". United States. https://doi.org/10.1039/c7fd00010c. https://www.osti.gov/servlets/purl/1436142.
@article{osti_1436142,
title = {Condensed-phase biogenic–anthropogenic interactions with implications for cold cloud formation},
author = {Charnawskas, Joseph C. and Alpert, Peter A. and Lambe, Andrew T. and Berkemeier, Thomas and O' Brien, Rachel E. and Massoli, Paola and Onasch, Timothy B. and Shiraiwa, Manabu and Moffet, Ryan C. and Gilles, Mary K. and Davidovits, Paul and Worsnop, Douglas R. and Knopf, Daniel A.},
abstractNote = {Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil-fuel combustion can acquire a coating of SOA. We investigate SOA-soot biogenic-anthropogenic interactions and their impact on ice nucleation in relation to the particles’ organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without presence of sulfate or soot particles. Corresponding particle glass transition (Tg) and full deliquescence relative humidity (FDRH) were estimated by a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfate mixtures exhibit a core-shell configuration (i.e. a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation in agreement with respective Tg and FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid inducing ice nucleation. Naphthalene SOA coated soot particles acted as IN above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not play a significant role in mixed-phase cloud formation and the presence of sulfate further renders this even less likely. Furthermore, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during preindustrial times or in pristine areas.},
doi = {10.1039/c7fd00010c},
journal = {Faraday Discussions},
number = ,
volume = 200,
place = {United States},
year = {Tue Jan 24 00:00:00 EST 2017},
month = {Tue Jan 24 00:00:00 EST 2017}
}
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Figures / Tables:
Table 1: Sample characteristics of biogenic SOA particles used in SEM images, ice nucleation experiments, and corresponding model simulations. The oxygen-to-carbon (O/C) ratio is a measurable surrogate of the SOA oxidation level. Tg,org is the glass transition temperature of the SOA under dry conditions. κ represents the hygroscopicity parameter. ρmore »
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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.