A diagonal volatility basis set to assess the condensation of organic vapors onto particles

We present a "diagonal" Volatility Basis Set (dVBS) comparing gas-phase concentrations of oxygenated organic molecules (OOM) to their condensed-phase mass fractions. This permits closure of vapor concentrations with particle composition constrained by particle growth rates, allowing the contributions of quasi non-volatile condensation, equilibrium partitioning, and reactive uptake to be separated. The dVBS accommodates both equilibrium and dynamical (growth) conditions. Growth implies an association between gas and particle concentrations governed by a "condensation line" that is set by the particle growth rate, which fixes the total (excess) concentration of condensible vapors. The condensation line defines an infeasible region of high particle mass fraction and low gas concentration; under steady-state growth conditions, compounds cannot appear in this infeasible region without being formed by condensed-phase chemistry. We test the dVBS with observations from the CLOUD experiment at CERN using data from a FIGAERO I<sup>-</sup> Chemical Ionization Mass Spectrometer measuring vapors directly and particle composition <i>via</i> temperature programmed desorption from a filter. A dVBS analysis finds that data from an α-pinene + O<sub>3</sub> run at 243 K are consistent with volatility driven condensation forming the large majority of particle mass, with no compounds clearly within the infeasible region.

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Publication Details

Journal
Environmental Science Atmospheres
Published
2025-01-01
DOI
https://doi.org/10.1039/d5ea00062a
Citations
3
Primary Topic
Atmospheric chemistry and aerosols
Type
article
Field-Weighted Citation Impact
3.90

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article

A diagonal volatility basis set to assess the condensation of organic vapors onto particles

Markku Kulmala, Roy L. Mauldin, J. Kirkby, Victoria Hofbauer et al.
3 citations
Environmental Science Atmospheres
Atmospheric chemistry and aerosols
3.90
article

A diagonal volatility basis set to assess the condensation of organic vapors onto particles

Markku Kulmala, Roy L. Mauldin, J. Kirkby, Victoria Hofbauer, Richard C. Flagan, Naser Mahfouz, Nirvan Bhattacharyya, Brandon Lopez, Katrianne Lehtipalo, Douglas R. Worsnop, Angela Buchholz, Siegfried Schobesberger, В. С. Махмутов, Meredith Schervish, Neil M. Donahue, Stefan K. Weber, Xu‐Cheng He, André Welti, Dominik Stolzenburg, Zoé Brasseur, Dexian Chen, Federico Bianchi, Mihnea Surdu, Ruby Marten, Imad El Haddad, Jonathan Duplissy, Maxim Philippov, Bernhard Mentler, Jenna DeVivo, Lucía Caudillo-Plath, Dongyu Wang, Mingyi Wang
article en
3 citations

Abstract

We present a "diagonal" Volatility Basis Set (dVBS) comparing gas-phase concentrations of oxygenated organic molecules (OOM) to their condensed-phase mass fractions. This permits closure of vapor concentrations with particle composition constrained by particle growth rates, allowing the contributions of quasi non-volatile condensation, equilibrium partitioning, and reactive uptake to be separated. The dVBS accommodates both equilibrium and dynamical (growth) conditions. Growth implies an association between gas and particle concentrations governed by a "condensation line" that is set by the particle growth rate, which fixes the total (excess) concentration of condensible vapors. The condensation line defines an infeasible region of high particle mass fraction and low gas concentration; under steady-state growth conditions, compounds cannot appear in this infeasible region without being formed by condensed-phase chemistry. We test the dVBS with observations from the CLOUD experiment at CERN using data from a FIGAERO I<sup>-</sup> Chemical Ionization Mass Spectrometer measuring vapors directly and particle composition <i>via</i> temperature programmed desorption from a filter. A dVBS analysis finds that data from an α-pinene + O<sub>3</sub> run at 243 K are consistent with volatility driven condensation forming the large majority of particle mass, with no compounds clearly within the infeasible region.

Environmental Science AtmospheresVol. 5(9)
Goethe University Frankfurt (DE), P.N. Lebedev Physical Institute of the Russian Academy of Sciences (RU), California Institute of Technology (US), Finnish Meteorological Institute (FI), University of Vienna (AT), University of Helsinki (FI), TU Wien (AT), Moscow Institute of Physics and Technology (RU), Sun Yat-sen University (CN), Cooperative Institute for Research in Environmental Sciences (US), University of Eastern Finland (FI), University of Colorado Boulder (US), Universität Innsbruck (AT), National Research University of Electronic Technology (RU), University of Cambridge (GB), Helsinki Institute of Physics (FI), Frankfurt Institute for Advanced Studies (DE), Paul Scherrer Institute (CH), Helsinki Institute for Information Technology (FI), University of Chicago (US), Institute of Physics and Technology (RU), Aerodyne Research (US), European Organization for Nuclear Research (CH), Carnegie Mellon University (US), National Research Nuclear University MEPhI (RU)
National Science Foundation, National Natural Science Foundation of China, Vienna Science and Technology Fund, Division of Chemistry
Openalex Percentile: Top 6%
Atmospheric chemistry and aerosols
3.90
DOIOpen Access PDFOpenAlex
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