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Title: The frequency-dependent response of single aerosol particles to vapour phase oscillations and its application in measuring diffusion coefficients

Abstract

A new method for measuring diffusion in the condensed phase of single aerosol particles is proposed and demonstrated. The technique is based on the frequency-dependent response of a binary particle to oscillations in the vapour phase of one of its chemical components. Here, we discuss how this physical situation allows for what would typically be a non-linear boundary value problem to be approximately reduced to a linear boundary value problem. For the case of aqueous aerosol particles, we investigate the accuracy of the closed-form analytical solution to this linear problem through a comparison with the numerical solution of the full problem. Then, using experimentally measured whispering gallery modes to track the frequency-dependent response of aqueous particles to relative humidity oscillations, we determine diffusion coefficients as a function of water activity. The measured diffusion coefficients are compared to previously reported values found using the two common experiments: (i) the analysis of the sorption/desorption of water from a particle after a step-wise change to the surrounding relative humidity and (ii) the isotopic exchange of water between a particle and the vapour phase. The technique presented here has two main strengths: first, when compared to the sorption/desorption experiment, it does not require themore » numerical evaluation of a boundary value problem during the fitting process as a closed-form expression is available. Second, when compared to the isotope exchange experiment, it does not require the use of labeled molecules. Therefore, the frequency-dependent experiment retains the advantages of these two commonly used methods but does not suffer from their drawbacks.« less

Authors:
ORCiD logo [1];  [2];  [2]
  1. McGill Univ., Montreal, QC (Canada). Dept. of Atmospheric and Oceanic Sciences and Dept. of Chemistry
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; Natural Sciences and Engineering Research Council of Canada (NSERC)
OSTI Identifier:
1454491
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP
Additional Journal Information:
Journal Volume: 19; Journal Issue: 5; Related Information: © 2017 the Owner Societies.; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 54 ENVIRONMENTAL SCIENCES

Citation Formats

Preston, Thomas C., Davies, James F., and Wilson, Kevin R. The frequency-dependent response of single aerosol particles to vapour phase oscillations and its application in measuring diffusion coefficients. United States: N. p., 2017. Web. doi:10.1039/c6cp07711k.
Preston, Thomas C., Davies, James F., & Wilson, Kevin R. The frequency-dependent response of single aerosol particles to vapour phase oscillations and its application in measuring diffusion coefficients. United States. https://doi.org/10.1039/c6cp07711k
Preston, Thomas C., Davies, James F., and Wilson, Kevin R. Fri . "The frequency-dependent response of single aerosol particles to vapour phase oscillations and its application in measuring diffusion coefficients". United States. https://doi.org/10.1039/c6cp07711k. https://www.osti.gov/servlets/purl/1454491.
@article{osti_1454491,
title = {The frequency-dependent response of single aerosol particles to vapour phase oscillations and its application in measuring diffusion coefficients},
author = {Preston, Thomas C. and Davies, James F. and Wilson, Kevin R.},
abstractNote = {A new method for measuring diffusion in the condensed phase of single aerosol particles is proposed and demonstrated. The technique is based on the frequency-dependent response of a binary particle to oscillations in the vapour phase of one of its chemical components. Here, we discuss how this physical situation allows for what would typically be a non-linear boundary value problem to be approximately reduced to a linear boundary value problem. For the case of aqueous aerosol particles, we investigate the accuracy of the closed-form analytical solution to this linear problem through a comparison with the numerical solution of the full problem. Then, using experimentally measured whispering gallery modes to track the frequency-dependent response of aqueous particles to relative humidity oscillations, we determine diffusion coefficients as a function of water activity. The measured diffusion coefficients are compared to previously reported values found using the two common experiments: (i) the analysis of the sorption/desorption of water from a particle after a step-wise change to the surrounding relative humidity and (ii) the isotopic exchange of water between a particle and the vapour phase. The technique presented here has two main strengths: first, when compared to the sorption/desorption experiment, it does not require the numerical evaluation of a boundary value problem during the fitting process as a closed-form expression is available. Second, when compared to the isotope exchange experiment, it does not require the use of labeled molecules. Therefore, the frequency-dependent experiment retains the advantages of these two commonly used methods but does not suffer from their drawbacks.},
doi = {10.1039/c6cp07711k},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 5,
volume = 19,
place = {United States},
year = {Fri Jan 13 00:00:00 EST 2017},
month = {Fri Jan 13 00:00:00 EST 2017}
}

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