Low-frequency depolarized Raman-spectral density of liquid water from femtosecond optical Kerr-effect measurements: Lineshape analysis of restricted translational modes

文献情報

出版日 2002-05-01

DOI 10.1039/B200299J

インパクトファクター 3.676

著者

Kathrin Winkler, Jörg Lindner, Peter Vöhringer

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要旨

A high-quality depolarized Raman-spectrum is obtained in the frequency range 0 ⩽ ω ⩽ 600 cm−1 by Fourier-transformation 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 fine 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.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

Low-frequency depolarized Raman-spectral density of liquid water from femtosecond optical Kerr-effect measurements: Lineshape analysis of restricted translational modes

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