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Development of simultaneous frequency- and time-resolved coherent anti-Stokes Raman scattering for ultrafast detection of molecular Raman spectra

J. Chem. Phys. 125, 044502 (2006); doi:10.1063/1.2219439

Published 24 July 2006

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Benjamin D. Prince, Abhijit Chakraborty, Beth M. Prince, and Hans U. Stauffer
Department of Chemistry, Iowa State University, Ames, Iowa 50011-3111
The development of a time-resolved coherent anti-Stokes Raman scattering (CARS) variant for use as a probe of excited electronic state Raman-active modes following excitation with an ultrafast pump pulse is detailed. Application of this technique involves a combination of broadband fs-time scale pulses and a narrowband pulse of ps duration that allows multiplexed detection of the CARS signal, permitting direct observation of molecular Raman frequencies and intensities with time resolution dictated by the broadband pulses. Thus, this nonlinear optical probe, designated fs/ps CARS, is suitable for observation of Raman spectral evolution following excitation with a pump pulse. Because of the spatial separation of the CARS output signal relative to the three input beams inherent in a folded BOXCARS arrangement, this technique is particularly amenable to probing low-frequency vibrational modes, which play a significant role in accepting vibrational energy during intramolecular vibrational energy redistribution within electronically excited states. Additionally, this spatial separation allows discrimination against strong fluorescence signal, as demonstrated in the case of rhodamine 6G. ©2006 American Institute of Physics
History: Received 24 August 2005; accepted 8 June 2006; published 24 July 2006
Permalink: http://link.aip.org/link/?JCPSA6/125/044502/1
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KEYWORDS and PACS

Keywords
PACS
  • 39.30.+w
    Spectroscopic techniques for atomic and molecular physics
  • 42.65.Dr
    Stimulated Raman scattering; CARS
  • 33.20.Fb
    Raman and Rayleigh molecular spectra including optical scattering
  • YEAR: 2006

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PUBLICATION DATA

ISSN:
0021-9606 (print)   1089-7690 (online)
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