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

Journal Article · · Physical Chemistry Chemical Physics. PCCP
DOI:https://doi.org/10.1039/c6cp07711k· OSTI ID:1454491
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
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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.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; Natural Sciences and Engineering Research Council of Canada (NSERC)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1454491
Journal Information:
Physical Chemistry Chemical Physics. PCCP, Vol. 19, Issue 5; Related Information: © 2017 the Owner Societies.; ISSN 1463-9076
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 12 works
Citation information provided by
Web of Science

References (37)

Secondary organic aerosol formation and transport journal September 1992
Water diffusion in atmospherically relevant α-pinene secondary organic material journal January 2015
A new approach to determine vapour pressures and hygroscopicities of aqueous aerosols containing semi-volatile organic compounds journal January 2014
The formation, properties and impact of secondary organic aerosol: current and emerging issues journal January 2009
The effect of viscosity and diffusion on the HO 2 uptake by sucrose and secondary organic aerosol particles journal January 2016
Drop-on-demand microdroplet generation: a very stable platform for single-droplet experimentation journal January 2016
Formation of Secondary Organic Aerosols Through Photooxidation of Isoprene journal February 2004
Gas/Particle Partitioning and Secondary Organic Aerosol Yields journal July 1996
Scattering of electromagnetic radiation by a multilayered sphere journal November 2009
Evolution of organic aerosol mass spectra upon heating: implications for OA phase and partitioning behavior journal January 2011
Phase of atmospheric secondary organic material affects its reactivity journal October 2012
Raman Spectroscopy of Isotopic Water Diffusion in Ultraviscous, Glassy, and Gel States in Aerosol by Use of Optical Tweezers journal January 2016
An amorphous solid state of biogenic secondary organic aerosol particles journal October 2010
Retrieving the translational diffusion coefficient of water from experiments on single levitated aerosol droplets journal January 2014
Variabilities and uncertainties in characterising water transport kinetics in glassy and ultraviscous aerosol journal January 2015
Accurate and efficient determination of the radius, refractive index, and dispersion of weakly absorbing spherical particle using whispering gallery modes journal January 2013
Secondary organic aerosol formation from anthropogenic air pollution: Rapid and higher than expected journal January 2006
Viscous organic aerosol particles in the upper troposphere: diffusivity-controlled water uptake and ice nucleation? journal January 2015
Laser-initiated iodine radical chemistry in single microdroplets journal November 2012
Models of Isotopic Water Diffusion in Spherical Aerosol Particles journal December 2016
Nanoscale interfacial gradients formed by the reactive uptake of OH radicals onto viscous aerosol surfaces journal January 2015
Quantifying water diffusion in high-viscosity and glassy aqueous solutions using a Raman isotope tracer method journal January 2014
Do atmospheric aerosols form glasses? journal January 2008
Exploring the complexity of aerosol particle properties and processes using single particle techniques journal January 2012
Influence of swelling and diffusion-induced convection on polymer sorption processes journal September 2002
Timescales of water transport in viscous aerosol: measurements on sub-micron particles and dependence on conditioning history journal January 2014
Comparing the mechanism of water condensation and evaporation in glassy aerosol journal July 2012
Raman- and Mie-Spectroscopic Studies of the Cooling Behaviour of Levitated, Single Sulfuric Acid/H2O Microdroplets journal June 2003
Ultra-slow water diffusion in aqueous sucrose glasses journal January 2011
Sucrose diffusion in aqueous solution journal January 2016
An absorption model of the gas/aerosol partitioning involved in the formation of secondary organic aerosol journal January 1994
Gas uptake and chemical aging of semisolid organic aerosol particles journal June 2011
Viscosity of  -pinene secondary organic material and implications for particle growth and reactivity journal April 2013
Chemistry of secondary organic aerosol: Formation and evolution of low-volatility organics in the atmosphere journal May 2008
Determining the size and refractive index of microspheres using the mode assignments from Mie resonances journal January 2015
Retrieval of the complex refractive index of aerosol droplets from optical tweezers measurements journal January 2012
Assessing the accuracy of complex refractive index retrievals from single aerosol particle cavity ring-down spectroscopy journal August 2016

Cited By (2)

Time evolution of steep diffusion fronts in highly viscous aerosol particles measured with Mie resonance spectroscopy journal December 2018
Time evolution of steep diffusion fronts in highly viscous aerosol particles measured with Mie resonance spectroscopy text January 2018

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