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ID: 17079.0, MPI für biophysikalische Chemie / Abteilungsunabhängige Arbeitsgruppen
Low-frequency depolarized Raman-spectral density of liquid water from femtosecond optical Kerr-effect measurements: Lineshape analysis of restricted translational modes
Authors:Winkler, K.; Lindner, J.; Voehringer, P.
Date of Publication (YYYY-MM-DD):2002
Title of Journal:Physical Chemistry Chemical Physics
Issue / Number:11
Start Page:2144
End Page:2155
Review Status:Peer-review
Audience:Not Specified
Abstract / Description:A high-quality depolarized Raman-spectrum is obtained in the frequency range 0 less than or equal to omega less than or equal to 600 cm(-1) by Fouriert-ransformation of time-resolved dual-color heterodyne-detected optical Kerr-effect data of liquid water at 0 C. The time-resolution was sufficient to fully capture the restricted translational and part of the hindered rotational region of the Raman spectrum. This low- temperature spectrum is used to test the applicability of stochastic line broadening theories. A conventional Kubo line shape analysis indicates that restricted translational modes involving hydrogen-bond bending and stretching motions are predominantly in the slow modulation limit at temperatures close to the melting point. However, a pronounced residual ne structure exists which cannot be fully accounted for by the theory in its standard form. Instead, we propose to apply a modified Kubo model based on truncating its continued-fraction representation at a finite order N including a convolution with a quasi-static structural inhomogeneity in the liquid. In particular, a quantitative agreement of our experimental data with such an inhomogeneous N-state random-jump model is interpreted with a discrete size distribution of aggregates which can interconvert on a time scale of about 500 fs by breaking and making of hydrogen bonds.
Comment of the Author/Creator:Date: 2002
External Publication Status:published
Document Type:Article
Communicated by:N. N.
Affiliations:MPI für biophysikalische Chemie/AG Peter Vöhringer
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