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Oxidation Enhances Aerosol Nucleation: Measurement of Kinetic Pickup Probability of Organic Molecules on Hydrated Acid Clusters
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    Oxidation Enhances Aerosol Nucleation: Measurement of Kinetic Pickup Probability of Organic Molecules on Hydrated Acid Clusters
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    • Jozef Lengyel*
      Jozef Lengyel
      Chair of Physical Chemistry, Department of Chemistry, Technical University of Munich, Lichtenbergstraße 4, 85748 Garching, Germany
      *E-mail: [email protected]
    • Andriy Pysanenko
      Andriy Pysanenko
      J. Heyrovský Institute of Physical Chemistry, v.v.i., Czech Academy of Sciences, Dolejškova 2155/3, 182 23 Prague, Czech Republic
    • Karolína Fárníková
      Karolína Fárníková
      J. Heyrovský Institute of Physical Chemistry, v.v.i., Czech Academy of Sciences, Dolejškova 2155/3, 182 23 Prague, Czech Republic
    • Eva Pluhařová*
      Eva Pluhařová
      J. Heyrovský Institute of Physical Chemistry, v.v.i., Czech Academy of Sciences, Dolejškova 2155/3, 182 23 Prague, Czech Republic
      *E-mail: [email protected]
    • Michal Fárník*
      Michal Fárník
      J. Heyrovský Institute of Physical Chemistry, v.v.i., Czech Academy of Sciences, Dolejškova 2155/3, 182 23 Prague, Czech Republic
      *E-mail: [email protected]
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    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2020, 11, 6, 2101–2105
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    https://doi.org/10.1021/acs.jpclett.0c00207
    Published February 26, 2020
    Copyright © 2020 American Chemical Society

    Abstract

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    We investigate the uptake of the most prominent biogenic volatile organic compounds (VOCs)—isoprene, α-pinene, and their selected oxidation products—by hydrated acid clusters in a molecular beam experiment and by DFT calculations. Our experiments provide a unique and direct way of determination of the surface accommodation coefficient (αS) on the proxies of ultrafine aerosol particles. Since we are able to determine unambiguously the fraction of the clusters to which the molecules stick upon collisions, our αS is a purely kinetic parameter disentangling the molecule pickup from its evaporation. Oxidation increases the αS of VOCs by more than an order of magnitude, because oxidized compounds form hydrogen bonds with the clusters, whereas the interactions of the parent VOCs are weaker and nonspecific. This work provides molecular-level insight into the condensation of single molecules into atmospheric particles, which has important implications for aerosol nucleation and growth.

    Copyright © 2020 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.0c00207.

    • Details of the experiment, theoretical calculations, and further results: mass spectra, velocity measurements, normalized pickup probabilities, relation to uptake coefficients, and calculated structures and binding energies (PDF)

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    Cited By

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    This article is cited by 11 publications.

    1. Michal Fárník. Bridging Gaps between Clusters in Molecular-Beam Experiments and Aerosol Nanoclusters. The Journal of Physical Chemistry Letters 2023, 14 (1) , 287-294. https://doi.org/10.1021/acs.jpclett.2c03417
    2. Leo Sala, Thomas F. M. Luxford, Miloš Ranković, Jaroslav Kočišek. Viewpoints on the 11th International Meeting on Atomic and Molecular Physics and Chemistry. The Journal of Physical Chemistry A 2022, 126 (46) , 8557-8561. https://doi.org/10.1021/acs.jpca.2c07768
    3. Ivo S. Vinklárek, Andriy Pysanenko, Eva Pluhařová, Michal Fárník. Uptake of Hydrogen Bonding Molecules by Benzene Nanoparticles. The Journal of Physical Chemistry Letters 2022, 13 (17) , 3781-3788. https://doi.org/10.1021/acs.jpclett.2c00835
    4. Matus E. Diveky, Michael J. Gleichweit, Sandra Roy, Ruth Signorell. Shining New Light on the Kinetics of Water Uptake by Organic Aerosol Particles. The Journal of Physical Chemistry A 2021, 125 (17) , 3528-3548. https://doi.org/10.1021/acs.jpca.1c00202
    5. Karolína Fárníková, Eva Pluhařová, Andrij Pysanenko, Michal Fárník, Yihui Yan, Jozef Lengyel. Dynamics of collisions and uptake of alcohol molecules with hydrated nitric acid clusters. Faraday Discussions 2024, 251 , 296-312. https://doi.org/10.1039/D3FD00160A
    6. Yadong Wang, Shiyu Zhan, Yongjun Hu, Xi Chen, Shi Yin. Understanding the Formation and Growth of New Atmospheric Particles at the Molecular Level through Laboratory Molecular Beam Experiments. ChemPlusChem 2024, 89 (7) https://doi.org/10.1002/cplu.202400108
    7. Kevin Li, Jozef Ďurana, Barbora Kocábková, Andrij Pysanenko, Yihui Yan, Milan Ončák, Michal Fárník, Jozef Lengyel. Hydrated Formic Acid Clusters and their Interaction with Electrons. ChemPhysChem 2024, 25 (10) https://doi.org/10.1002/cphc.202400071
    8. Andriy Pysanenko, Karolína Fárníková, Jozef Lengyel, Eva Pluhařová, Michal Fárník. Molecular-level insight into uptake of dimethylamine on hydrated nitric acid clusters. Environmental Science: Atmospheres 2022, 2 (6) , 1292-1302. https://doi.org/10.1039/D2EA00094F
    9. Andriy Pysanenko, Ivo S. Vinklárek, Michal Fárník, Viktoriya Poterya. Generation of (H2O2)N clusters on argon and ice nanoparticles. International Journal of Mass Spectrometry 2021, 461 , 116514. https://doi.org/10.1016/j.ijms.2020.116514
    10. Michal Fárník, Juraj Fedor, Jaroslav Kočišek, Jozef Lengyel, Eva Pluhařová, Viktoriya Poterya, Andriy Pysanenko. Pickup and reactions of molecules on clusters relevant for atmospheric and interstellar processes. Physical Chemistry Chemical Physics 2021, 23 (5) , 3195-3213. https://doi.org/10.1039/D0CP06127A
    11. Mithlesh Mahilang, Manas Kanti Deb, Shamsh Pervez. Biogenic secondary organic aerosols: A review on formation mechanism, analytical challenges and environmental impacts. Chemosphere 2021, 262 , 127771. https://doi.org/10.1016/j.chemosphere.2020.127771

    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2020, 11, 6, 2101–2105
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.0c00207
    Published February 26, 2020
    Copyright © 2020 American Chemical Society

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