Ultrafast memory loss and energy redistribution in the hydrogen bond network of liquid H2O

  title={Ultrafast memory loss and energy redistribution in the hydrogen bond network of liquid H2O},
  author={Michael L. Cowan and Barry D Bruner and Nils Huse and Jason R. Dwyer and Brige P. Chugh and Erik T J Nibbering and Thomas Elsaesser and R. J. Dwayne Miller},
Many of the unusual properties of liquid water are attributed to its unique structure, comprised of a random and fluctuating three-dimensional network of hydrogen bonds that link the highly polar water molecules. One of the most direct probes of the dynamics of this network is the infrared spectrum of the OH stretching vibration, which reflects the distribution of hydrogen-bonded structures and the intermolecular forces controlling the structural dynamics of the liquid. Indeed, water dynamics… Expand
Anharmonic exciton dynamics and energy dissipation in liquid water from two-dimensional infrared spectroscopy.
This paper presents a comprehensive analysis of the two-dimensional infrared spectrum of O-H stretching vibrations in liquid H2O and their interactions with bending and intermolecular vibrations and argues that the collective nature of water vibrations should be considered in describing aqueous solvation. Expand
Molecular dynamics simulation of nonlinear spectroscopies of intermolecular motions in liquid water.
These theoretical methods do not require frequently used assumptions and can thus be called ab initio methods; together with multidimensional nonlinear spectroscopies, they provide powerful methods for examining the inter- and intramolecular details of water dynamics. Expand
Hydrogen bond reorganization and vibrational relaxation in water studied with ultrafast infrared spectroscopy
Water consists of an extended hydrogen bond network that is constantly evolving. More than just a description of the time averaged structure is necessary to understand any process that occurs inExpand
Ultrafast memory loss and relaxation processes in hydrogen-bonded systems
Vibrational spectroscopy in the femtosecond time domain is applied to map structural dynamics in real-time and identify underlying molecular interactions in an aqueous environment that displays an ultrafast loss of structural memory. Expand
Femtosecond mid-infrared study of the reorientation of weakly hydrogen-bonded water molecules.
It is observed that with increasing temperature, the spectral relaxation shows a similar acceleration as the average molecular reorientation, showing that these processes are intimately connected. Expand
Multidimensional infrared spectroscopy of water. I. Vibrational dynamics in two-dimensional IR line shapes.
The modeling based on fluctuations with Gaussian statistics is able to reproduce the changes in dispersed pump-probe and 2D IR spectra induced by these relaxation processes, but misses the asymmetry resulting from frequency-dependent spectral diffusion. Expand
Energy transfer within the hydrogen bonding network of water following resonant terahertz excitation
The dynamic energy flow in the hydrogen bond network of liquid water is investigated by a pump-probe experiment that resonantly excites intermolecular degrees of freedom with ultrashort single-cycle terahertz pulses and monitors its Raman response. Expand
Structural rearrangements in water viewed through two-dimensional infrared spectroscopy.
This Account reviews recent ultrafast 2D IR studies at MIT that provide new information on the mechanism of hydrogen-bond rearrangements in liquid water, and demonstrates a more general, unique characteristic of the spectroscopy: if a spectral signature of the transition state exists, then 2DIR can effectively serve as a transition-state spectroscope. Expand
Two-dimensional infrared spectroscopy of intermolecular hydrogen bonds in the condensed phase.
  • T. Elsaesser
  • Chemistry, Medicine
  • Accounts of chemical research
  • 2009
This Account reviews recent progress originating from third-order nonlinear methods of coherent multidimensional vibrational spectroscopy and expects that the application of 2D infrared Spectroscopy in an extended spectral range will reveal the intrinsic coupling between water and specific functional units of DNA. Expand
Ultrafast intermolecular dynamics of liquid water: a theoretical study on two-dimensional infrared spectroscopy.
The present result reveals that the anharmonic coupling between the hindered translation and libration motions is essential for the ultrafast relaxation dynamics in liquid water. Expand


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