Structure from Dynamics: Vibrational Dynamics of Interfacial Water as a Probe of Aqueous Heterogeneity

The Journal of Physical Chemistry. B
Jenée D CyranMischa Bonn

Abstract

The structural heterogeneity of water at various interfaces can be revealed by time-resolved sum-frequency generation spectroscopy. The vibrational dynamics of the O-H stretch vibration of interfacial water can reflect structural variations. Specifically, the vibrational lifetime is typically found to increase with increasing frequency of the O-H stretch vibration, which can report on the hydrogen-bonding heterogeneity of water. We compare and contrast vibrational dynamics of water in contact with various surfaces, including vapor, biomolecules, and solid interfaces. The results reveal that variations in the vibrational lifetime with vibrational frequency are very typical, and can frequently be accounted for by the bulk-like heterogeneous response of interfacial water. Specific interfaces exist, however, for which the behavior is less straightforward. These insights into the heterogeneity of interfacial water thus obtained contribute to a better understanding of complex phenomena taking place at aqueous interfaces, such as photocatalytic reactions and protein folding.

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Citations

Apr 30, 2020·Physical Chemistry Chemical Physics : PCCP·Malte DeiserothEllen H G Backus
Mar 15, 2020·Annual Review of Chemical and Biomolecular Engineering·Jacob MonroeM Scott Shell
Sep 11, 2020·Proceedings of the National Academy of Sciences of the United States of America·Haoyuan WangWei Xiong
Sep 15, 2020·Physical Chemistry Chemical Physics : PCCP·Abhinav SrivastavaAnanya Debnath
Oct 8, 2020·Proceedings of the National Academy of Sciences of the United States of America·Nan YangMark A Johnson
Aug 20, 2019·Journal of Colloid and Interface Science·Jean-François BoilyHongfei Wang
Mar 20, 2021·The Journal of Physical Chemistry. B·Andrew P CarpenterGeraldine L Richmond
Jan 15, 2021·Annual Review of Physical Chemistry·Haoyuan Wang, Wei Xiong
Oct 28, 2019·The Journal of Physical Chemistry Letters·Takakazu SekiYuki Nagata
Apr 6, 2019·The Journal of Physical Chemistry. C, Nanomaterials and Interfaces·Shumei SunEllen H G Backus
Nov 9, 2018·The Journal of Physical Chemistry Letters·Sanghamitra SenguptaEric Tyrode
Dec 17, 2020·The Journal of Physical Chemistry. B·Christopher P BaryiamesCarlos R Baiz
Dec 1, 2020·Nano Letters·Sayantan Mondal, Biman Bagchi

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