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Laser-induced gratings in free jets. III. Saturation-induced anharmonic gratings

Journal Article · · Journal of Chemical Physics; (United States)
DOI:https://doi.org/10.1063/1.466568· OSTI ID:5429050
;  [1]
  1. Combustion Research Facility, Sandia National Laboratories, Livermore, California 94551 (United States)
We apply two-color laser-induced grating spectroscopy (LIGS) to obtain excitation spectra of the [ital S][sub 1]([ital [tilde A]] [sup 1][ital B][sub 1])--[ital S][sub 0]([ital [tilde X]] [sup 1][ital A][sub 1]) system of jet-cooled azulene. The ground-state depletion grating created by excitation with crossed beams is probed via either the [ital S][sub 2]([ital [tilde B]] [sup 1][ital A][sub 1])--[ital S][sub 0]([ital [tilde X]] [sup 1][ital A][sub 1]) or [ital S][sub 4]([ital [tilde D]] [sup 1][ital A][sub 1])--[ital S][sub 0]([ital [tilde X]] [sup 1][ital A][sub 1]) transitions. First-order LIGS spectra of the [ital S][sub 1]--[ital S][sub 0] origin band at several grating-laser intensities reveal saturation-induced line broadening and significant saturation dips at line center. We develop a simple model, based on the anharmonic grating created in the saturated regime, and use it to fit the first-order data. From these fits we determine a saturation parameter and the linewidth of the [ital S][sub 1]--[ital S][sub 0] origin absorption band, which is homogeneously broadened due to rapid internal conversion ([tau][similar to]1 ps) in the [ital S][sub 1] state. We also observe LIGS spectra of the azulene origin taken at the second Bragg order of the induced grating; the observed second-order lineshapes are also fit with the anharmonic-grating model.
OSTI ID:
5429050
Journal Information:
Journal of Chemical Physics; (United States), Journal Name: Journal of Chemical Physics; (United States) Vol. 100:2; ISSN JCPSA6; ISSN 0021-9606
Country of Publication:
United States
Language:
English