Timescales of secondary organic aerosols to reach equilibrium at various temperatures and relative humidities
Abstract
Abstract. Secondary organic aerosols (SOA) account for a substantial fraction of air particulate matter, and SOA formation is often modeled assuming rapid establishment of gas–particle equilibrium. Here, we estimate the characteristic timescale for SOA to achieve gas–particle equilibrium under a wide range of temperatures and relative humidities using a state-of-the-art kinetic flux model. Equilibration timescales were calculated by varying particle phase state, size, mass loadings, and volatility of organic compounds in open and closed systems. Model simulations suggest that the equilibration timescale for semi-volatile compounds is on the order of seconds or minutes for most conditions in the planetary boundary layer, but it can be longer than 1 h if particles adopt glassy or amorphous solid states with high glass transition temperatures at low relative humidity. In the free troposphere with lower temperatures, it can be longer than hours or days, even at moderate or relatively high relative humidities due to kinetic limitations of bulk diffusion in highly viscous particles. The timescale of partitioning of low-volatile compounds into highly viscous particles is shorter compared to semi-volatile compounds in the closed system, as it is largely determined by condensation sink due to very slow re-evaporation with relatively quick establishment of local equilibrium betweenmore »
- Authors:
- Publication Date:
- Research Org.:
- Univ. of California, Irvine, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC); National Science Foundation (NSF)
- OSTI Identifier:
- 1511101
- Alternate Identifier(s):
- OSTI ID: 1612951
- Grant/Contract Number:
- SC0018349; AGS-1654104
- Resource Type:
- Published Article
- Journal Name:
- Atmospheric Chemistry and Physics (Online)
- Additional Journal Information:
- Journal Name: Atmospheric Chemistry and Physics (Online) Journal Volume: 19 Journal Issue: 9; Journal ID: ISSN 1680-7324
- Publisher:
- Copernicus Publications, EGU
- Country of Publication:
- Germany
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES; environmental sciences & ecology; meteorology & atmospheric Sciences
Citation Formats
Li, Ying, and Shiraiwa, Manabu. Timescales of secondary organic aerosols to reach equilibrium at various temperatures and relative humidities. Germany: N. p., 2019.
Web. doi:10.5194/acp-19-5959-2019.
Li, Ying, & Shiraiwa, Manabu. Timescales of secondary organic aerosols to reach equilibrium at various temperatures and relative humidities. Germany. https://doi.org/10.5194/acp-19-5959-2019
Li, Ying, and Shiraiwa, Manabu. Tue .
"Timescales of secondary organic aerosols to reach equilibrium at various temperatures and relative humidities". Germany. https://doi.org/10.5194/acp-19-5959-2019.
@article{osti_1511101,
title = {Timescales of secondary organic aerosols to reach equilibrium at various temperatures and relative humidities},
author = {Li, Ying and Shiraiwa, Manabu},
abstractNote = {Abstract. Secondary organic aerosols (SOA) account for a substantial fraction of air particulate matter, and SOA formation is often modeled assuming rapid establishment of gas–particle equilibrium. Here, we estimate the characteristic timescale for SOA to achieve gas–particle equilibrium under a wide range of temperatures and relative humidities using a state-of-the-art kinetic flux model. Equilibration timescales were calculated by varying particle phase state, size, mass loadings, and volatility of organic compounds in open and closed systems. Model simulations suggest that the equilibration timescale for semi-volatile compounds is on the order of seconds or minutes for most conditions in the planetary boundary layer, but it can be longer than 1 h if particles adopt glassy or amorphous solid states with high glass transition temperatures at low relative humidity. In the free troposphere with lower temperatures, it can be longer than hours or days, even at moderate or relatively high relative humidities due to kinetic limitations of bulk diffusion in highly viscous particles. The timescale of partitioning of low-volatile compounds into highly viscous particles is shorter compared to semi-volatile compounds in the closed system, as it is largely determined by condensation sink due to very slow re-evaporation with relatively quick establishment of local equilibrium between the gas phase and the near-surface bulk. The dependence of equilibration timescales on both volatility and bulk diffusivity provides critical insights into thermodynamic or kinetic treatments of SOA partitioning for accurate predictions of gas- and particle-phase concentrations of semi-volatile compounds in regional and global chemical transport models.},
doi = {10.5194/acp-19-5959-2019},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 9,
volume = 19,
place = {Germany},
year = {Tue May 07 00:00:00 EDT 2019},
month = {Tue May 07 00:00:00 EDT 2019}
}
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