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Complexity of Measuring and Representing the Hygroscopicity of Mixed Component Aerosol

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Original languageEnglish
Pages (from-to)1648-1660
Number of pages13
JournalJournal of Physical Chemistry A
Volume123
Issue number8
Early online date1 Feb 2019
DOIs
DateAccepted/In press - 1 Feb 2019
DateE-pub ahead of print - 1 Feb 2019
DatePublished (current) - 28 Feb 2019

Abstract

The validation of approaches to predict the hygroscopicity of complex mixtures of organic components in aerosol is important for understanding the hygroscopic response of organic aerosol in the atmosphere. We report new measurements of the hygroscopicity of mixtures of dicarboxylic acids and amino acids using a comparative kinetic electrodynamic balance (CK-EDB) approach, inferring the equilibrium water content of the aerosol from close to a saturation relative humidity (100 %) down to 80 %. We show that the solution densities and refractive indices of the mixtures can be estimated with an accuracy of better than ±2 % using the molar refractive index mixing rule and densities and refractive indices for the individual binary organic-aqueous solutions. Further, we show that the often-used mass, volume and mole-weighted mixing rules to estimate the hygroscopicity parameter  can over-estimate the hygroscopic parameter by a factor of as much as 3, highlighting the need to understand the specific non-ideal interactions that may arise synergistically in mixtures and cannot be represented by simple models. Indeed, in some extreme cases the hygroscopicity of a multicomponent mixture can be very close to that for the least hygroscopic component. For mixtures of similar components for which no additional synergistic interactions need be considered, the hygroscopicity of the mixed component aerosol can be estimated with high accuracy from the hygroscopic response of the binary aqueous-organic aerosol. In conclusion, we suggest that the hygroscopicity of multicomponent organic aerosol can be highly non-additive and that simple correlations of hygroscopicity with composition may often misrepresent the level of complexity essential to interpret aerosol hygroscopicity.

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    Rights statement: This is the author accepted manuscript (AAM). The final published version (version of record) is available online via ACS at https://pubs.acs.org/doi/10.1021/acs.jpca.8b11623 . Please refer to any applicable terms of use of the publisher.

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