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Two-dimensional Raman-terahertz spectroscopy of water


Savolainen, J; Ahmed, S; Hamm, P (2013). Two-dimensional Raman-terahertz spectroscopy of water. Proceedings of the National Academy of Sciences of the United States of America, 110(51):20402-20407.

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.

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.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Language:English
Date:2013
Deposited On:16 Jan 2014 14:28
Last Modified:05 Apr 2016 17:22
Publisher:National Academy of Sciences
ISSN:0027-8424
Funders:Swiss National Science Foundation (SNF) through the NCCR MUST
Free access at:Publisher DOI. An embargo period may apply.
Publisher DOI:https://doi.org/10.1073/pnas.1317459110
PubMed ID:24297930

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