TY - JOUR
T1 - Accurate Prediction of Organic Aerosol Evaporation Using Kinetic Multilayer Modeling and the Stokes-Einstein Equation
AU - Ingram, Stephen
AU - Rovelli, Grazia
AU - Song, Young Chul
AU - Topping, David
AU - Dutcher, Cari S.
AU - Liu, Shihao
AU - Nandy, Lucy
AU - Shiraiwa, Manabu
AU - Reid, Jonathan P.
N1 - Publisher Copyright:
© 2021 American Chemical Society. All rights reserved.
PY - 2021/4/29
Y1 - 2021/4/29
N2 - Organic aerosol can adopt a wide range of viscosities, from liquid to glass, depending on the local humidity. In highly viscous droplets, the evaporation rates of organic components are suppressed to varying degrees, yet water evaporation remains fast. Here, we examine the coevaporation of semivolatile organic compounds (SVOCs), along with their solvating water, from aerosol particles levitated in a humidity-controlled environment. To better replicate the composition of secondary aerosol, nonvolatile organics were also present, creating a three-component diffusion problem. Kinetic modeling reproduced the evaporation accurately when the SVOCs were assumed to obey the Stokes-Einstein relation, and water was not. Crucially, our methodology uses previously collected data to constrain the time-dependent viscosity, as well as water diffusion coefficients, allowing it to be predictive rather than postdictive. Throughout the study, evaporation rates were found to decrease as SVOCs deplete from the particle, suggesting path function type behavior.
AB - Organic aerosol can adopt a wide range of viscosities, from liquid to glass, depending on the local humidity. In highly viscous droplets, the evaporation rates of organic components are suppressed to varying degrees, yet water evaporation remains fast. Here, we examine the coevaporation of semivolatile organic compounds (SVOCs), along with their solvating water, from aerosol particles levitated in a humidity-controlled environment. To better replicate the composition of secondary aerosol, nonvolatile organics were also present, creating a three-component diffusion problem. Kinetic modeling reproduced the evaporation accurately when the SVOCs were assumed to obey the Stokes-Einstein relation, and water was not. Crucially, our methodology uses previously collected data to constrain the time-dependent viscosity, as well as water diffusion coefficients, allowing it to be predictive rather than postdictive. Throughout the study, evaporation rates were found to decrease as SVOCs deplete from the particle, suggesting path function type behavior.
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U2 - 10.1021/acs.jpca.1c00986
DO - 10.1021/acs.jpca.1c00986
M3 - Article
C2 - 33861595
AN - SCOPUS:85105038061
SN - 1089-5639
VL - 125
SP - 3444
EP - 3456
JO - Journal of Physical Chemistry A
JF - Journal of Physical Chemistry A
IS - 16
ER -