Comparative OHD-RIKES and THz-TDS probes of ultrafast structural dynamics in molecular liquids

Matthew C. Beard; William T. Lotshaw; Timothy M. Korter; Edwin J. Heilweil; Dale McMorrow

doi:10.1021/jp047547a

Comparative OHD-RIKES and THz-TDS probes of ultrafast structural dynamics in molecular liquids

Matthew C. Beard, William T. Lotshaw, Timothy M. Korter, Edwin J. Heilweil, Dale McMorrow

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23 Scopus citations

Abstract

We compare terahertz time domain (THz-TDS) and optical heterodyne-detected Raman-induced Kerr effect (OHD-RIKES) spectroscopic techniques as probes of molecular and vibrational dynamics in the frequency range of 0.1 to 6 THz (3 to 200 cm ^-1). The spectra of molecular liquids benzene, toluene, and bromobenzene, with dipole moments in the range of 0 to 1.7 D, are analyzed within a multimode spectral decomposition to examine the relative sensitivities of the techniques to distinguishable dynamical coordinates. We emphasize the use of minimum modal bases primarily for the purpose of comparing the spectra. Significant differences are found between the THz and OHD-RIKES spectra of benzene and bromobenzene that cannot be traced to rescaled oscillator strengths within a set of fixed-frequency modes.

Original language	English (US)
Pages (from-to)	9348-9360
Number of pages	13
Journal	Journal of Physical Chemistry A
Volume	108
Issue number	43
DOIs	https://doi.org/10.1021/jp047547a
State	Published - Oct 28 2004

ASJC Scopus subject areas

Physical and Theoretical Chemistry

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abstract = "We compare terahertz time domain (THz-TDS) and optical heterodyne-detected Raman-induced Kerr effect (OHD-RIKES) spectroscopic techniques as probes of molecular and vibrational dynamics in the frequency range of 0.1 to 6 THz (3 to 200 cm -1). The spectra of molecular liquids benzene, toluene, and bromobenzene, with dipole moments in the range of 0 to 1.7 D, are analyzed within a multimode spectral decomposition to examine the relative sensitivities of the techniques to distinguishable dynamical coordinates. We emphasize the use of minimum modal bases primarily for the purpose of comparing the spectra. Significant differences are found between the THz and OHD-RIKES spectra of benzene and bromobenzene that cannot be traced to rescaled oscillator strengths within a set of fixed-frequency modes.",

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AU - Beard, Matthew C.

AU - Lotshaw, William T.

AU - Korter, Timothy M.

AU - Heilweil, Edwin J.

AU - McMorrow, Dale

PY - 2004/10/28

Y1 - 2004/10/28

N2 - We compare terahertz time domain (THz-TDS) and optical heterodyne-detected Raman-induced Kerr effect (OHD-RIKES) spectroscopic techniques as probes of molecular and vibrational dynamics in the frequency range of 0.1 to 6 THz (3 to 200 cm -1). The spectra of molecular liquids benzene, toluene, and bromobenzene, with dipole moments in the range of 0 to 1.7 D, are analyzed within a multimode spectral decomposition to examine the relative sensitivities of the techniques to distinguishable dynamical coordinates. We emphasize the use of minimum modal bases primarily for the purpose of comparing the spectra. Significant differences are found between the THz and OHD-RIKES spectra of benzene and bromobenzene that cannot be traced to rescaled oscillator strengths within a set of fixed-frequency modes.

AB - We compare terahertz time domain (THz-TDS) and optical heterodyne-detected Raman-induced Kerr effect (OHD-RIKES) spectroscopic techniques as probes of molecular and vibrational dynamics in the frequency range of 0.1 to 6 THz (3 to 200 cm -1). The spectra of molecular liquids benzene, toluene, and bromobenzene, with dipole moments in the range of 0 to 1.7 D, are analyzed within a multimode spectral decomposition to examine the relative sensitivities of the techniques to distinguishable dynamical coordinates. We emphasize the use of minimum modal bases primarily for the purpose of comparing the spectra. Significant differences are found between the THz and OHD-RIKES spectra of benzene and bromobenzene that cannot be traced to rescaled oscillator strengths within a set of fixed-frequency modes.

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Comparative OHD-RIKES and THz-TDS probes of ultrafast structural dynamics in molecular liquids

Abstract

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