Condensed-phase biogenic–anthropogenic interactions with implications for cold cloud formation

Author:

Charnawskas Joseph C.12345,Alpert Peter A.12345,Lambe Andrew T.67859,Berkemeier Thomas1011125,O’Brien Rachel E.131415516,Massoli Paola9175,Onasch Timothy B.67859ORCID,Shiraiwa Manabu1618195,Moffet Ryan C.1620215,Gilles Mary K.1314155,Davidovits Paul6785,Worsnop Douglas R.9175,Knopf Daniel A.12345ORCID

Affiliation:

1. Institute for Terrestrial and Planetary Atmospheres

2. School of Marine and Atmospheric Sciences

3. Stony Brook University

4. Stony Brook

5. USA

6. Chemistry Department

7. Boston College

8. Chestnut Hill

9. Aerodyne Research Inc.

10. School of Chemical and Biomolecular Engineering

11. Georgia Institute of Technology

12. Atlanta

13. Chemical Sciences Division

14. Lawrence Berkeley National Laboratory

15. Berkeley

16. Department of Chemistry

17. Billerica

18. University of California

19. Irvine

20. University of the Pacific

21. Stockton

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 the presence of sulfate or soot particles. Corresponding particle glass transition (Tg) and full deliquescence relative humidity (FDRH) were estimated using 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 respectiveTgand 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 ice nuclei 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 renders this even less likely. However, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during pre-industrial times or in pristine areas.

Funder

Division of Atmospheric and Geospace Sciences

Biological and Environmental Research

Basic Energy Sciences

Publisher

Royal Society of Chemistry (RSC)

Subject

Physical and Theoretical Chemistry

Reference132 articles.

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