We have studied the temperature dependence of the vibrational frequency fluctuation of the antisymmetric stretching mode of in by three-pulse infrared (IR) photon echo experiments. IR pump-probe measurements were also carried out to investigate the population relaxation and the orientational relaxation of the same band. It was found that the time-correlation function (TCF) of the frequency fluctuation of this mode is well described by a biexponential function with a quasistatic term. The faster decay component has a time constant of about 0.1 ps, and the slower component varies from 1.4 to 1.1 ps in the temperature range from 283 to 353 K. This result indicates that liquid dynamics related to the frequency fluctuation are not highly sensitive to temperature. We discuss the relationship between the temperature dependence of the vibrational frequency fluctuation and that of the molecular motion of the system to investigate the molecular origin of the frequency fluctuation of the solute. We compare the temperature dependence of the frequency fluctuation with that of other dynamics such as dielectric relaxation of water. In contrast to the Debye dielectric relaxation time of , the two time constants of the TCF of the frequency fluctuation do not exhibit strong temperature dependence. We propose a simple theoretical model for the frequency fluctuation in solutions based on perturbation theory and the dipole-dipole interaction between the vibrational mode of the solute and the solvent molecules. This model suggests that the neighboring solvent molecules in the vicinity of the solute play an important role in the frequency fluctuation. We suggest that the picosecond component of the frequency fluctuation results from structural fluctuation of the hydrogen-bonding network in water.
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7 July 2010
Research Article|
July 07 2010
Temperature dependence of vibrational frequency fluctuation of in
Jumpei Tayama;
Jumpei Tayama
1Graduate School of Science,
Kobe University
, Nada, Kobe 657-8501, Japan
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Akane Ishihara;
Akane Ishihara
1Graduate School of Science,
Kobe University
, Nada, Kobe 657-8501, Japan
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Motohiro Banno;
Motohiro Banno
2Molecular Photoscience Research Center,
Kobe University
, Nada, Kobe 657-8501, Japan
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Kaoru Ohta;
Kaoru Ohta
3PRESTO,
JST
, 4-1-8 Honcho Kawaguchi, Saitama 332-0012, Japan
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Shinji Saito;
Shinji Saito
4
Institute for Molecular Science
, Myodaiji, Okazaki 444-8585, Japan
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Keisuke Tominaga
Keisuke Tominaga
a)
1Graduate School of Science,
Kobe University
, Nada, Kobe 657-8501, Japan
2Molecular Photoscience Research Center,
Kobe University
, Nada, Kobe 657-8501, Japan
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Jumpei Tayama
1
Akane Ishihara
1
Motohiro Banno
2
Kaoru Ohta
3
Shinji Saito
4
Keisuke Tominaga
1,2,a)
1Graduate School of Science,
Kobe University
, Nada, Kobe 657-8501, Japan
2Molecular Photoscience Research Center,
Kobe University
, Nada, Kobe 657-8501, Japan
3PRESTO,
JST
, 4-1-8 Honcho Kawaguchi, Saitama 332-0012, Japan
4
Institute for Molecular Science
, Myodaiji, Okazaki 444-8585, Japan
a)
Electronic mail: [email protected]. Tel.: +81-78-803-5684. FAX: +81-78-803-5684.
J. Chem. Phys. 133, 014505 (2010)
Article history
Received:
December 28 2009
Accepted:
April 21 2010
Citation
Jumpei Tayama, Akane Ishihara, Motohiro Banno, Kaoru Ohta, Shinji Saito, Keisuke Tominaga; Temperature dependence of vibrational frequency fluctuation of in . J. Chem. Phys. 7 July 2010; 133 (1): 014505. https://doi.org/10.1063/1.3428672
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