Nonlinear response functions for birefringence and dichroism measurements in condensed phases

Minhaeng Cho, Graham R. Fleming, Shaul Mukamel

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The fourth-rank tensorial nonlinear response function which controls the response of a chromophore in the condensed phase to three arbitrarily polarized external fields is calculated. Internal (vibrational and rotational) degrees of freedom are incorporated using wave packets in Liouville space (the doorway/window picture). The rotational contribution of the chromophore is expressed in terms of a conditional probability for the rotational diffusion model. We apply this formalism to transient dichroism and birefringence spectroscopies.

Original languageEnglish
Pages (from-to)5314-5326
Number of pages13
JournalThe Journal of Chemical Physics
Issue number7
Publication statusPublished - 1993 Dec 1
Externally publishedYes


ASJC Scopus subject areas

  • Atomic and Molecular Physics, and Optics

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