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Coherent X-rays reveal the influence of cage effects on ultrafast water dynamics

Author

Listed:
  • Fivos Perakis

    (Stockholm University
    SLAC National Accelerator Laboratory)

  • Gaia Camisasca

    (Stockholm University)

  • Thomas J. Lane

    (SLAC National Accelerator Laboratory)

  • Alexander Späh

    (Stockholm University)

  • Kjartan Thor Wikfeldt

    (Stockholm University)

  • Jonas A. Sellberg

    (AlbaNova University Center, KTH Royal Institute of Technology)

  • Felix Lehmkühler

    (Deutsches Elektronen-Synchrotron DESY
    Hamburg Centre for Ultrafast Imaging)

  • Harshad Pathak

    (Stockholm University)

  • Kyung Hwan Kim

    (Stockholm University)

  • Katrin Amann-Winkel

    (Stockholm University)

  • Simon Schreck

    (Stockholm University)

  • Sanghoon Song

    (SLAC National Accelerator Laboratory)

  • Takahiro Sato

    (SLAC National Accelerator Laboratory)

  • Marcin Sikorski

    (SLAC National Accelerator Laboratory
    European XFEL)

  • Andre Eilert

    (SLAC National Accelerator Laboratory)

  • Trevor McQueen

    (SLAC National Accelerator Laboratory)

  • Hirohito Ogasawara

    (SLAC National Accelerator Laboratory)

  • Dennis Nordlund

    (SLAC National Accelerator Laboratory)

  • Wojciech Roseker

    (Deutsches Elektronen-Synchrotron DESY)

  • Jake Koralek

    (SLAC National Accelerator Laboratory)

  • Silke Nelson

    (SLAC National Accelerator Laboratory)

  • Philip Hart

    (SLAC National Accelerator Laboratory)

  • Roberto Alonso-Mori

    (SLAC National Accelerator Laboratory)

  • Yiping Feng

    (SLAC National Accelerator Laboratory)

  • Diling Zhu

    (SLAC National Accelerator Laboratory)

  • Aymeric Robert

    (SLAC National Accelerator Laboratory)

  • Gerhard Grübel

    (Deutsches Elektronen-Synchrotron DESY
    Hamburg Centre for Ultrafast Imaging)

  • Lars G. M. Pettersson

    (Stockholm University)

  • Anders Nilsson

    (Stockholm University)

Abstract

The dynamics of liquid water feature a variety of time scales, ranging from extremely fast ballistic-like thermal motion, to slower molecular diffusion and hydrogen-bond rearrangements. Here, we utilize coherent X-ray pulses to investigate the sub-100 fs equilibrium dynamics of water from ambient conditions down to supercooled temperatures. This novel approach utilizes the inherent capability of X-ray speckle visibility spectroscopy to measure equilibrium intermolecular dynamics with lengthscale selectivity, by measuring oxygen motion in momentum space. The observed decay of the speckle contrast at the first diffraction peak, which reflects tetrahedral coordination, is attributed to motion on a molecular scale within the first 120 fs. Through comparison with molecular dynamics simulations, we conclude that the slowing down upon cooling from 328 K down to 253 K is not due to simple thermal ballistic-like motion, but that cage effects play an important role even on timescales over 25 fs due to hydrogen-bonding.

Suggested Citation

  • Fivos Perakis & Gaia Camisasca & Thomas J. Lane & Alexander Späh & Kjartan Thor Wikfeldt & Jonas A. Sellberg & Felix Lehmkühler & Harshad Pathak & Kyung Hwan Kim & Katrin Amann-Winkel & Simon Schreck , 2018. "Coherent X-rays reveal the influence of cage effects on ultrafast water dynamics," Nature Communications, Nature, vol. 9(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-04330-5
    DOI: 10.1038/s41467-018-04330-5
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