Theoretical description of the vibrational echo spectroscopy by time-resolved infrared-infrared-visible difference-frequency generation

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Abstract

Theoretical descriptions of the time-resolved infrared-infrared visible (IIV) sum and difference frequency generation are presented. The IIV sum-frequency generation (SFG) method is shown to be useful in selectively studying the vibrational relaxation of the overtone mode. The IIV difference-frequency generation (DFG), which is a specific case of the doubly resonant four-wave mixing spectroscopies, involves a rephasing period so that the elimination of the vibrational inhomogeneous broadening can be achieved by using this method. The decay of the diagonal IIV-DFG signal is proven to be independent on the inhomogeneous distribution of the vibrational frequency. Furthermore, it is shown that the two-dimensional time-resolved IIV-DFG signal along the antidiagonal provides a direct information on the vibrational inhomogeneous distribution function.

Original languageEnglish
Pages (from-to)10587-10594
Number of pages8
JournalJournal of Chemical Physics
Volume111
Issue number23
Publication statusPublished - 1999 Dec 15

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echoes
Spectroscopy
Infrared radiation
spectroscopy
molecular relaxation
four-wave mixing
elimination
distribution functions
Four wave mixing
harmonics
Vibrational spectra
Distribution functions
decay

ASJC Scopus subject areas

  • Atomic and Molecular Physics, and Optics

Cite this

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title = "Theoretical description of the vibrational echo spectroscopy by time-resolved infrared-infrared-visible difference-frequency generation",
abstract = "Theoretical descriptions of the time-resolved infrared-infrared visible (IIV) sum and difference frequency generation are presented. The IIV sum-frequency generation (SFG) method is shown to be useful in selectively studying the vibrational relaxation of the overtone mode. The IIV difference-frequency generation (DFG), which is a specific case of the doubly resonant four-wave mixing spectroscopies, involves a rephasing period so that the elimination of the vibrational inhomogeneous broadening can be achieved by using this method. The decay of the diagonal IIV-DFG signal is proven to be independent on the inhomogeneous distribution of the vibrational frequency. Furthermore, it is shown that the two-dimensional time-resolved IIV-DFG signal along the antidiagonal provides a direct information on the vibrational inhomogeneous distribution function.",
author = "Minhaeng Cho",
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AU - Cho, Minhaeng

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N2 - Theoretical descriptions of the time-resolved infrared-infrared visible (IIV) sum and difference frequency generation are presented. The IIV sum-frequency generation (SFG) method is shown to be useful in selectively studying the vibrational relaxation of the overtone mode. The IIV difference-frequency generation (DFG), which is a specific case of the doubly resonant four-wave mixing spectroscopies, involves a rephasing period so that the elimination of the vibrational inhomogeneous broadening can be achieved by using this method. The decay of the diagonal IIV-DFG signal is proven to be independent on the inhomogeneous distribution of the vibrational frequency. Furthermore, it is shown that the two-dimensional time-resolved IIV-DFG signal along the antidiagonal provides a direct information on the vibrational inhomogeneous distribution function.

AB - Theoretical descriptions of the time-resolved infrared-infrared visible (IIV) sum and difference frequency generation are presented. The IIV sum-frequency generation (SFG) method is shown to be useful in selectively studying the vibrational relaxation of the overtone mode. The IIV difference-frequency generation (DFG), which is a specific case of the doubly resonant four-wave mixing spectroscopies, involves a rephasing period so that the elimination of the vibrational inhomogeneous broadening can be achieved by using this method. The decay of the diagonal IIV-DFG signal is proven to be independent on the inhomogeneous distribution of the vibrational frequency. Furthermore, it is shown that the two-dimensional time-resolved IIV-DFG signal along the antidiagonal provides a direct information on the vibrational inhomogeneous distribution function.

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