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Quantum State-Resolved Energy Transfer Dynamics at Gas−Liquid Interfaces:  IR Laser Studies of CO2 Scattering from Perfluorinated Liquids

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    Quantum State-Resolved Energy Transfer Dynamics at Gas−Liquid Interfaces:  IR Laser Studies of CO2 Scattering from Perfluorinated Liquids
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    JILA, University of Colorado and National Institute of Standards and Technology, and Department of Chemistry and Biochemistry, University of Colorado, Boulder, Colorado 80309-0440
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    The Journal of Physical Chemistry B

    Cite this: J. Phys. Chem. B 2005, 109, 34, 16396–16405
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    https://doi.org/10.1021/jp0511404
    Published August 5, 2005
    Copyright © 2005 American Chemical Society
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    Abstract

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    An apparatus for detailed study of quantum state-resolved inelastic energy transfer dynamics at the gas−liquid interface is described. The approach relies on supersonic jet-cooled molecular beams impinging on a continuously renewable liquid surface in a vacuum and exploits sub-Doppler high-resolution laser absorption methods to probe rotational, vibrational, and translational distributions in the scattered flux. First results are presented for skimmed beams of jet-cooled CO2 (Tbeam ≈ 15 K) colliding at normal incidence with a liquid perfluoropolyether (PFPE) surface at Einc = 10.6(8) kcal/mol. The experiment uses a tunable Pb-salt diode laser for direct absorption on the CO2 ν3 asymmetric stretch. Measured rotational distributions in both 0000 and 01 10 vibrational manifolds indicate CO2 inelastically scatters from the liquid surface into a clearly non-Boltzmann distribution, revealing nonequilibrium dynamics with average rotational energies in excess of the liquid (Ts = 300 K). Furthermore, high-resolution analysis of the absorption profiles reveals that Doppler widths correspond to temperatures significantly warmer than Ts and increase systematically with the J rotational state. These rotational and translational distributions are consistent with two distinct gas−liquid collision pathways:  (i) a T ≈ 300 K component due to trapping-desorption (TD) and (ii) a much hotter distribution (T ≈ 750 K) due to “prompt” impulsive scattering (IS) from the gas−liquid interface. By way of contrast, vibrational populations in the CO2 bending mode are inefficiently excited by scattering from the liquid, presumably reflecting much slower T−V collisional energy transfer rates.

    Copyright © 2005 American Chemical Society

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    †

     Present address:  Radiant Dyes Laser, Wermelskirchen, Germany.

    *

     Corresponding author. E-mail:  [email protected].

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    The Journal of Physical Chemistry B

    Cite this: J. Phys. Chem. B 2005, 109, 34, 16396–16405
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jp0511404
    Published August 5, 2005
    Copyright © 2005 American Chemical Society
    Request reuse permissions

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