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.
N1 - Publisher Copyright:
© 2021 American Chemical Society.
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
UR - http://www.scopus.com/inward/record.url?scp=85119402569&partnerID=8YFLogxK
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 -