Modeling the Size Distribution and Chemical Composition of Secondary Organic Aerosols during the Reactive Uptake of Isoprene-Derived Epoxydiols under Low-Humidity Condition

Mega Octaviani; Manish Shrivastava; Rahul A. Zaveri; Alla Zelenyuk; Yue Zhang; Quazi Z. Rasool; David M. Bell; Matthieu Riva; Marianne Glasius; Jason D. Surratt

doi:10.1021/acsearthspacechem.1c00303

Modeling the Size Distribution and Chemical Composition of Secondary Organic Aerosols during the Reactive Uptake of Isoprene-Derived Epoxydiols under Low-Humidity Condition

Mega Octaviani, Manish Shrivastava^*, Rahul A. Zaveri, Alla Zelenyuk, Yue Zhang, Quazi Z. Rasool, David M. Bell, Matthieu Riva, Marianne Glasius, Jason D. Surratt

^*Corresponding author for this work

Department of Chemistry

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

8 Citations (Scopus)

Abstract

Reactive uptake of isoprene epoxydiols (IEPOX), which are isoprene oxidation products, onto acidic sulfate aerosols is recognized to be an important mechanism for the formation of isoprene-derived secondary organic aerosol (SOA). While a mechanistic understanding of IEPOX-SOA formation exists, several processes affecting their formation remain uncertain. Evaluating mechanistic IEPOX-SOA models with controlled laboratory experiments under longer atmospherically relevant time scales is critical. Here, we implement our latest understanding of IEPOX-SOA formation within a box model to simulate the measured reactive uptake of IEPOX on polydisperse ammonium bisulfate seed aerosols within an environmental Teflon chamber. The model is evaluated with single-particle measurements of size distribution, volume, density, and composition of aerosols due to IEPOX-SOA formation at time scales of hours. We find that the model can simulate the growth of particles due to IEPOX multiphase chemistry, as reflected in increases of the mean particle size and volume concentrations, and a shift of the number size distribution to larger sizes. The model also predicts the observed evolution of particle number mean diameter and total volume concentrations at the end of the experiment. We show that in addition to the self-limiting effects of IEPOX-SOA coatings, the mass accommodation coefficient of IEPOX and accounting for the molar balance between inorganic and organic sulfate are important parameters governing the modeling of the IEPOX-SOA formation. Thus, models which do not account for the molar sulfate balance and/or diffusion limitations within IEPOX-SOA coatings are likely to predict IEPOX-SOA formation too high.

Original language	English
Journal	ACS Earth and Space Chemistry
Volume	5
Issue	11
Pages (from-to)	3247-3257
Number of pages	11
ISSN	2472-3452
DOIs	https://doi.org/10.1021/acsearthspacechem.1c00303
Publication status	Published - Nov 2021

Keywords

box modeling
chamber measurements
chemical composition
isoprene epoxydiols
low relative humidity
multiphase chemistry
secondary organic aerosols
size distribution

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10.1021/acsearthspacechem.1c00303

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Octaviani, M., Shrivastava, M., Zaveri, R. A., Zelenyuk, A., Zhang, Y., Rasool, Q. Z., Bell, D. M., Riva, M., Glasius, M., & Surratt, J. D. (2021). Modeling the Size Distribution and Chemical Composition of Secondary Organic Aerosols during the Reactive Uptake of Isoprene-Derived Epoxydiols under Low-Humidity Condition. ACS Earth and Space Chemistry, 5(11), 3247-3257. https://doi.org/10.1021/acsearthspacechem.1c00303

@article{19de9ad1c5f14becaa80cda213e1ec08,

title = "Modeling the Size Distribution and Chemical Composition of Secondary Organic Aerosols during the Reactive Uptake of Isoprene-Derived Epoxydiols under Low-Humidity Condition",

abstract = "Reactive uptake of isoprene epoxydiols (IEPOX), which are isoprene oxidation products, onto acidic sulfate aerosols is recognized to be an important mechanism for the formation of isoprene-derived secondary organic aerosol (SOA). While a mechanistic understanding of IEPOX-SOA formation exists, several processes affecting their formation remain uncertain. Evaluating mechanistic IEPOX-SOA models with controlled laboratory experiments under longer atmospherically relevant time scales is critical. Here, we implement our latest understanding of IEPOX-SOA formation within a box model to simulate the measured reactive uptake of IEPOX on polydisperse ammonium bisulfate seed aerosols within an environmental Teflon chamber. The model is evaluated with single-particle measurements of size distribution, volume, density, and composition of aerosols due to IEPOX-SOA formation at time scales of hours. We find that the model can simulate the growth of particles due to IEPOX multiphase chemistry, as reflected in increases of the mean particle size and volume concentrations, and a shift of the number size distribution to larger sizes. The model also predicts the observed evolution of particle number mean diameter and total volume concentrations at the end of the experiment. We show that in addition to the self-limiting effects of IEPOX-SOA coatings, the mass accommodation coefficient of IEPOX and accounting for the molar balance between inorganic and organic sulfate are important parameters governing the modeling of the IEPOX-SOA formation. Thus, models which do not account for the molar sulfate balance and/or diffusion limitations within IEPOX-SOA coatings are likely to predict IEPOX-SOA formation too high. ",

keywords = "box modeling, chamber measurements, chemical composition, isoprene epoxydiols, low relative humidity, multiphase chemistry, secondary organic aerosols, size distribution",

author = "Mega Octaviani and Manish Shrivastava and Zaveri, {Rahul A.} and Alla Zelenyuk and Yue Zhang and Rasool, {Quazi Z.} and Bell, {David M.} and Matthieu Riva and Marianne Glasius and Surratt, {Jason D.}",

note = "Publisher Copyright: {\textcopyright} 2021 American Chemical Society.",

year = "2021",

month = nov,

doi = "10.1021/acsearthspacechem.1c00303",

language = "English",

volume = "5",

pages = "3247--3257",

journal = "ACS Earth and Space Chemistry",

issn = "2472-3452",

publisher = "American Chemical Society",

number = "11",

}

Octaviani, M, Shrivastava, M, Zaveri, RA, Zelenyuk, A, Zhang, Y, Rasool, QZ, Bell, DM, Riva, M, Glasius, M & Surratt, JD 2021, 'Modeling the Size Distribution and Chemical Composition of Secondary Organic Aerosols during the Reactive Uptake of Isoprene-Derived Epoxydiols under Low-Humidity Condition', ACS Earth and Space Chemistry, vol. 5, no. 11, pp. 3247-3257. https://doi.org/10.1021/acsearthspacechem.1c00303

Modeling the Size Distribution and Chemical Composition of Secondary Organic Aerosols during the Reactive Uptake of Isoprene-Derived Epoxydiols under Low-Humidity Condition. / Octaviani, Mega; Shrivastava, Manish; Zaveri, Rahul A. et al.
In: ACS Earth and Space Chemistry, Vol. 5, No. 11, 11.2021, p. 3247-3257.

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

TY - JOUR

T1 - Modeling the Size Distribution and Chemical Composition of Secondary Organic Aerosols during the Reactive Uptake of Isoprene-Derived Epoxydiols under Low-Humidity Condition

AU - Octaviani, Mega

AU - Shrivastava, Manish

AU - Zaveri, Rahul A.

AU - Zelenyuk, Alla

AU - Zhang, Yue

AU - Rasool, Quazi Z.

AU - Bell, David M.

AU - Riva, Matthieu

AU - Glasius, Marianne

AU - Surratt, Jason D.

PY - 2021/11

Y1 - 2021/11

N2 - Reactive uptake of isoprene epoxydiols (IEPOX), which are isoprene oxidation products, onto acidic sulfate aerosols is recognized to be an important mechanism for the formation of isoprene-derived secondary organic aerosol (SOA). While a mechanistic understanding of IEPOX-SOA formation exists, several processes affecting their formation remain uncertain. Evaluating mechanistic IEPOX-SOA models with controlled laboratory experiments under longer atmospherically relevant time scales is critical. Here, we implement our latest understanding of IEPOX-SOA formation within a box model to simulate the measured reactive uptake of IEPOX on polydisperse ammonium bisulfate seed aerosols within an environmental Teflon chamber. The model is evaluated with single-particle measurements of size distribution, volume, density, and composition of aerosols due to IEPOX-SOA formation at time scales of hours. We find that the model can simulate the growth of particles due to IEPOX multiphase chemistry, as reflected in increases of the mean particle size and volume concentrations, and a shift of the number size distribution to larger sizes. The model also predicts the observed evolution of particle number mean diameter and total volume concentrations at the end of the experiment. We show that in addition to the self-limiting effects of IEPOX-SOA coatings, the mass accommodation coefficient of IEPOX and accounting for the molar balance between inorganic and organic sulfate are important parameters governing the modeling of the IEPOX-SOA formation. Thus, models which do not account for the molar sulfate balance and/or diffusion limitations within IEPOX-SOA coatings are likely to predict IEPOX-SOA formation too high.

AB - Reactive uptake of isoprene epoxydiols (IEPOX), which are isoprene oxidation products, onto acidic sulfate aerosols is recognized to be an important mechanism for the formation of isoprene-derived secondary organic aerosol (SOA). While a mechanistic understanding of IEPOX-SOA formation exists, several processes affecting their formation remain uncertain. Evaluating mechanistic IEPOX-SOA models with controlled laboratory experiments under longer atmospherically relevant time scales is critical. Here, we implement our latest understanding of IEPOX-SOA formation within a box model to simulate the measured reactive uptake of IEPOX on polydisperse ammonium bisulfate seed aerosols within an environmental Teflon chamber. The model is evaluated with single-particle measurements of size distribution, volume, density, and composition of aerosols due to IEPOX-SOA formation at time scales of hours. We find that the model can simulate the growth of particles due to IEPOX multiphase chemistry, as reflected in increases of the mean particle size and volume concentrations, and a shift of the number size distribution to larger sizes. The model also predicts the observed evolution of particle number mean diameter and total volume concentrations at the end of the experiment. We show that in addition to the self-limiting effects of IEPOX-SOA coatings, the mass accommodation coefficient of IEPOX and accounting for the molar balance between inorganic and organic sulfate are important parameters governing the modeling of the IEPOX-SOA formation. Thus, models which do not account for the molar sulfate balance and/or diffusion limitations within IEPOX-SOA coatings are likely to predict IEPOX-SOA formation too high.

KW - box modeling

KW - chamber measurements

KW - chemical composition

KW - isoprene epoxydiols

KW - low relative humidity

KW - multiphase chemistry

KW - secondary organic aerosols

KW - size distribution

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U2 - 10.1021/acsearthspacechem.1c00303

DO - 10.1021/acsearthspacechem.1c00303

M3 - Journal article

AN - SCOPUS:85119402569

SN - 2472-3452

VL - 5

SP - 3247

EP - 3257

JO - ACS Earth and Space Chemistry

JF - ACS Earth and Space Chemistry

IS - 11

ER -

Modeling the Size Distribution and Chemical Composition of Secondary Organic Aerosols during the Reactive Uptake of Isoprene-Derived Epoxydiols under Low-Humidity Condition

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