Off-resonant coherent hyper-Raman scattering spectroscopy

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Abstract

A theoretical description of the off-resonant coherent hyper-Raman scattering spectroscopy is presented. By considering two pump fields whose frequencies and corresponding wave vectors are ω1, ω2(= 2ω1), k1, and k2, respectively, the effective Hamiltonian is derived to show that the spatial transient grating can be created by the third-order interaction with the pump fields. A delayed probe field with frequency of ω1 and wave vector of k1 is scattered by the spatial transient grating to produce the macroscopic polarization with wave vector 4k1 - k2. The expressions for the measured signals by homodyne and heterodyne method are derived and compared with that of the spontaneous hyper-Raman scattering signal.

Original languageEnglish
Pages (from-to)7550-7557
Number of pages8
JournalJournal of Chemical Physics
Volume106
Issue number18
DOIs
Publication statusPublished - 1997 May 8

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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