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Theory for determination of the low-frequency time-dependent response function in liquids using time-resolved terahertz pulse spectroscopy

J. Chem. Phys. 110, 8589 (1999); doi:10.1063/1.478766

Issue Date: 1 May 1999

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James T. Kindt and Charles A. Schmuttenmaer
Department of Chemistry, Yale University, New Haven, Connecticut 06520-8107
With the current rapid improvement in techniques for generating and detecting femtosecond terahertz (fs-THz) pulses, it is now possible to detect time-dependent perturbations to low-frequency intermolecular far-infrared modes during solvation events. The interpretation of these time-resolved terahertz spectroscopy experiments has generally relied on a collapse of the information available in the fs-THz pulse to give a one-dimensional time-dependent function, whose physical significance is not well defined. We describe a method to exploit the full electric field profile of the pulse as a function of pump/probe delay time to obtain a two-dimensional function that describes the system's time-dependent dielectric response. We discuss the physical significance of this response function in terms of the time evolution of solute/solvent modes following photoexcitation, and give examples to show how its qualitative features relate to the measurable signal. ©1999 American Institute of Physics.
History: Received 8 December 1998; accepted 5 February 1999
Permalink: http://link.aip.org/link/?JCPSA6/110/8589/1
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KEYWORDS and PACS

Keywords
PACS
  • 78.30.Cp
    Optical properties, condensed-matter spectroscopy and other interactions of radiation and particles with condensed matter Infrared and Raman spectra Liquids
  • 78.47.+p
    Optical properties, condensed-matter spectroscopy and other interactions of radiation and particles with condensed matter Time-resolved optical spectroscopies and other ultrafast optical measurements in condensed matter
  • 82.30.Nr
    Physical chemistry Specific chemical reactions; reaction mechanisms Association, addition, insertion, cluster formation, hydrogen bonding
  • YEAR: 1999

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PUBLICATION DATA

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