Direct Observation of Ultrafast Hydrogen Bond Strengthening in Liquid Water

Yang, Jie

doi:10.1038/s41586-021-03793-9

Direct Observation of Ultrafast Hydrogen Bond Strengthening in Liquid Water

Journal Article · Fri Jan 01 00:00:00 EST 2021 · Nature (London)

DOI:https://doi.org/10.1038/s41586-021-03793-9· OSTI ID:1798809

Yang, Jie ^[1]

SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); SLAC

Water is one of the most important, yet least understood, liquids in nature. Many anomalous properties of liquid water originate from its well-connected hydrogen bond network, including unusually efficient vibrational energy redistribution and relaxation. An accurate description of the ultrafast vibrational motion of water molecules is essential for understanding the nature of hydrogen bonds and many solution-phase chemical reactions. Most existing knowledge of vibrational relaxation in water is built upon ultrafast spectroscopy experiments. However, these experiments cannot directly resolve the motion of the atomic positions and require difficult translation of spectral dynamics into hydrogen bond dynamics. Here we measured the ultrafast structural response to the excitation of the OH stretching vibration in liquid water with femtosecond temporal and atomic spatial resolution using liquid ultrafast electron scattering. We observed a transient hydrogen bond contraction of roughly 0.04 Å on a timescale of 80 femtoseconds, followed by a thermalization on a timescale of ~1 picosecond. Molecular dynamics simulations reveal the need to treat the distribution of the shared proton in the hydrogen bond quantum mechanically to capture the structural dynamics on the femtosecond timescales. Our experiment and simulations unveiled the intermolecular character of the water vibration preceding the relaxation of the OH stretch.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515; SC0014170

OSTI ID:: 1798809

Alternate ID(s):: OSTI ID: 1819310

Journal Information:: Nature (London), Journal Name: Nature (London) Journal Issue: 7873 Vol. 596; ISSN 0028-0836

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Dataset for "Direct Observation of Ultrafast Hydrogen Bond Strengthening in Liquid Water" Yang, Jie; Dettori, Riccardo; F. Nunes, J. Pedro Zenodo https://doi.org/10.5281/zenodo.4048936	dataset	January 2020
How van der Waals interactions determine the unique properties of water Morawietz, Tobias; Singraber, Andreas; Dellago, Christoph figshare https://doi.org/10.6084/m9.figshare.1497907	dataset	January 2015

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