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

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, Sanghoon Song, Takahiro Sato, Marcin Sikorski, Andre Eilert, Trevor McQueen, Hirohito Ogasawara, Dennis Nordlund, Wojciech Roseker, Jake Koralek, Silke Nelson, Philip Hart, Roberto Alonso-Mori, Yiping Feng, Diling Zhu, Aymeric Robert, Gerhard Grübel, Lars G. M. Pettersson and Anders Nilsson ()
Additional contact information
Fivos Perakis: Stockholm University
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
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
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
Lars G. M. Pettersson: Stockholm University
Anders Nilsson: Stockholm University

Nature Communications, 2018, vol. 9, issue 1, 1-10

Abstract: 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.

Date: 2018
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DOI: 10.1038/s41467-018-04330-5

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