Nonequilibrium Behavior in Isoprene Secondary Organic Aerosol

Chen, Yuzhi; Zaveri, Rahul A.; Vandergrift, Gregory W.; Cheng, Zezhen; China, Swarup; Zelenyuk, Alla; Shilling, John E.

doi:10.1021/acs.est.3c03532

Title: Nonequilibrium Behavior in Isoprene Secondary Organic Aerosol

Journal Article · 14 September 2023 · Environmental Science and Technology

DOI: https://doi.org/10.1021/acs.est.3c03532 · OSTI ID:2203048

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Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Recent studies have shown that instantaneous gas-particle equilibrium partitioning assumptions fail to predict SOA formation, even at high relative humidity (~85%), and photochemical aging seems to be one driving factor. In this study, we probe the minimum aging time scale required to observe nonequilibrium partitioning of semivolatile organic compounds (SVOCs) between the gas and aerosol phase at ~50% RH. Seed isoprene SOA is generated by photo-oxidation in the presence of effloresced ammonium sulfate seeds at <1 ppbv NO_x, aged photochemically or in the dark for 0.3–6 h, and subsequently exposed to fresh isoprene SVOCs. Our results show that the equilibrium partitioning assumption is accurate for fresh isoprene SOA but breaks down after isoprene SOA has been aged for as short as 20 min even in the dark. Modeling results show that a semisolid SOA phase state is necessary to reproduce the observed particle size distribution evolution. The observed nonequilibrium partitioning behavior and inferred semisolid phase state are corroborated by offline mass spectrometric analysis on the bulk aerosol particles showing the formation of organosulfates and oligomers. Here, the unexpected short time scale for the phase transition within isoprene SOA has important implications for the growth of atmospheric ultrafine particles to climate-relevant sizes.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Atmospheric Radiation Measurement (ARM) Data Center; Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Contributing Organization:: Pacific Northwest National Laboratory (PNNL); Brookhaven National Laboratory (BNL); Argonne National Laboratory (ANL); Oak Ridge National Laboratory (ORNL)

Grant/Contract Number:: AC06-76RL01830; AC05-76RL01830

OSTI ID:: 2203048

Alternate ID(s):: OSTI ID: 2203049

Report Number(s):: PNNL-SA-185113

Journal Information:: Environmental Science and Technology, Vol. 57, Issue 38; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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54 ENVIRONMENTAL SCIENCES
isoprene
secondary organic aerosol (SOA)
equilibrium partitioning
diffusion limitations
aerosols
equilibrium
nanoparticles
phase transitions
physiology

Title: Nonequilibrium Behavior in Isoprene Secondary Organic Aerosol

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