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Theory of femtosecond stimulated Raman spectroscopy

J. Chem. Phys. 121, 3632 (2004); doi:10.1063/1.1777214

Issue Date: 22 August 2004

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Soo-Y. Lee and Donghui Zhang
Department of Chemistry, National University of Singapore, Kent Ridge, Singapore 117543, Singapore

David W. McCamant, Philipp Kukura, and Richard A. Mathies
Department of Chemistry, University of California, Berkeley, California 94720
Femtosecond broadband stimulated Raman spectroscopy (FSRS) is a new technique that produces high-resolution (time-resolved) vibrational spectra from either the ground or excited electronic states of molecules, free from background fluorescence. FSRS uses simultaneously a narrow bandwidth ~1–3 ps Raman pump pulse with a continuum ~30–50 fs Stokes probe pulse to produce sharp Raman gains, at positions corresponding to vibrational transitions in the sample, riding on top of the continuum Stokes probe spectrum. When FSRS is preceded by a femtosecond actinic pump pulse that initiates the photochemistry of interest, time-resolved Raman spectroscopy can be carried out. We present two theoretical approaches to FSRS: one is based on a coupling of Raman pump and probe light waves with the vibrations in the medium, and another is a quantum-mechanical description. The latter approach is used to discuss the conditions of applicability and limitations of the coupled-wave description. Extension of the quantum-mechanical description to the case where the Raman pump beam is on resonance with an excited electronic state, as well as when FSRS is used to probe a nonstationary vibrational wave packet prepared by an actinic pump pulse, is also discussed. ©2004 American Institute of Physics.
History: Received 23 April 2004; accepted 7 June 2004
Permalink: http://link.aip.org/link/?JCPSA6/121/3632/1
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KEYWORDS and PACS

Keywords
PACS
  • 33.20.Tp
    Vibrational analysis (molecular spectra)
  • 33.20.Fb
    Raman and Rayleigh molecular spectra including optical scattering
  • 39.30.+w
    Spectroscopic techniques for atomic and molecular physics
  • 33.80.Be
    Molecular level crossing and optical pumping
  • 03.65.-w
    Quantum mechanics
  • YEAR: 2004

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PUBLICATION DATA

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