Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 105, Issue 35, Pages 12684-12689Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.0800401105
Keywords
alignment; impulsive scattering; liquid surface; orientation; trapping-desorption
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Funding
- Air Force Office of Scientific Research
- National Science Foundation
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Stereodynamics at the gas-liquid interface provides insight into the important physical interactions that directly influence heterogeneous chemistry at the surface and within the bulk liquid. We investigate molecular beam scattering Of CO2 from a liquid perfluoropolyether (PFPE) surface in vacuum [incident energy E-inc = 10.6(8) kcal/mol, incident angle theta(inc) = 60 degrees] to specifically reveal rotational angular-momentum directions for scattered molecules. Experimentally, internal quantum state populations and M-J distributions are probed by high-resolution polarization-modulated infrared laser spectroscopy. Analysis of J-state populations reveals dual-channel scattering dynamics characterized by a two-temperature Boltzmann distribution for trapping-desorption and impulsive scattering. In addition, molecular dynamics simulations of CO2 + fluorinated self-assembled monolayers have been used to model CO2 + PFPE dynamics. Experimental results and molecular dynamics simulations reveal highly oriented CO2 distributions that preferentially scatter with top spin as a strongly increasing function of J state.
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