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Two-dimensional Raman-terahertz spectroscopy of water.


ABSTRACT: Two-dimensional Raman-terahertz (THz) spectroscopy is presented as a multidimensional spectroscopy directly in the far-IR regime. The method is used to explore the dynamics of the collective intermolecular modes of liquid water at ambient temperatures that emerge from the hydrogen-bond networks water forming. Two-dimensional Raman-THz spectroscopy interrogates these modes twice and as such can elucidate couplings and inhomogeneities of the various degrees of freedoms. An echo in the 2D Raman-THz response is indeed identified, indicating that a heterogeneous distribution of hydrogen-bond networks exists, albeit only on a very short 100-fs timescale. This timescale appears to be too short to be compatible with more extended, persistent structures assumed within a two-state model of water.

SUBMITTER: Savolainen J 

PROVIDER: S-EPMC3870715 | biostudies-literature | 2013 Dec

REPOSITORIES: biostudies-literature

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Two-dimensional Raman-terahertz spectroscopy of water.

Savolainen Janne J   Ahmed Saima S   Hamm Peter P  

Proceedings of the National Academy of Sciences of the United States of America 20131202 51


Two-dimensional Raman-terahertz (THz) spectroscopy is presented as a multidimensional spectroscopy directly in the far-IR regime. The method is used to explore the dynamics of the collective intermolecular modes of liquid water at ambient temperatures that emerge from the hydrogen-bond networks water forming. Two-dimensional Raman-THz spectroscopy interrogates these modes twice and as such can elucidate couplings and inhomogeneities of the various degrees of freedoms. An echo in the 2D Raman-THz  ...[more]

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