Chemical identification of new particle formation and growth precursors through positive matrix factorization of ambient ion measurements

Katz, Daniel John; Abdelhamid, Aroob; Stark, Harald; Canagaratna, Manjula R.; Worsnop, Douglas R.; Browne, Eleanor C.

doi:10.5194/acp-23-5567-2023

Chemical identification of new particle formation and growth precursors through positive matrix factorization of ambient ion measurements

Journal Article · Wed May 17 04:00:00 EDT 2023 · Atmospheric Chemistry and Physics (Online)

DOI:https://doi.org/10.5194/acp-23-5567-2023· OSTI ID:1974082

; Abdelhamid, Aroob; Stark, Harald; Canagaratna, Manjula R.; Worsnop, Douglas R.;

Abstract. In the lower troposphere, rapid collisions between ions and trace gases result in the transfer of positive charge to the highest proton affinity species and negative charge to the lowest proton affinity species. Measurements of the chemical composition of ambient ions thus provide direct insight into the most acidic and basic trace gases and their ion–molecule clusters – compounds thought to be important for new particle formation and growth. We deployed an atmospheric pressure interface time-of-flight mass spectrometer (APi-ToF) to measure ambient ion chemical composition during the 2016 Holistic Interactions of Shallow Clouds, Aerosols, and Land Ecosystems (HI-SCALE) campaign at the United States Department of Energy Atmospheric Radiation Measurement facility in the Southern Great Plains (SGP), an agricultural region. Cations and anions were measured for alternating periods of ∼ 24 h over 1 month. We use binned positive matrix factorization (binPMF) and generalized Kendrick analysis (GKA) to obtain information about the chemical formulas and temporal variation in ionic composition without the need for averaging over a long timescale or a priori high-resolution peak fitting. Negative ions consist of strong acids including sulfuric and nitric acid, organosulfates, and clusters of NO3- with highly oxygenated organic molecules (HOMs) derived from monoterpene (MT) and sesquiterpene (SQT) oxidation. Organonitrates derived from SQTs account for most of the HOM signal. Combined with the diel profiles and back trajectory analysis, these results suggest that NO3 radical chemistry is active at this site. SQT oxidation products likely contribute to particle growth at the SGP site. The positive ions consist of bases including alkyl pyridines and amines and a series of high-mass species. Nearly all the positive ions contained only one nitrogen atom and in general support ammonia and amines as being the dominant bases that could participate in new particle formation. Overall, this work demonstrates how APi-ToF measurements combined with binPMF analysis can provide insight into the temporal evolution of compounds important for new particle formation and growth.

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

Grant/Contract Number:: SC0011218; SC0020175

OSTI ID:: 1974082

Alternate ID(s):: OSTI ID: 1975278
OSTI ID: 1976108

Journal Information:: Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Journal Issue: 9 Vol. 23; ISSN 1680-7324

Publisher:: Copernicus GmbHCopyright Statement

Country of Publication:: Germany

Language:: English

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Multiple new-particle growth pathways observed at the US DOE Southern Great Plains field site

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