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

Nature Communications
Fivos PerakisAnders Nilsson

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.

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Citations

Apr 16, 2019·Philosophical Transactions. Series A, Mathematical, Physical, and Engineering Sciences·Thorsten Bartels-Rausch, Maurine Montagnat
Sep 7, 2019·Journal of Synchrotron Radiation·Johannes MöllerAnders Madsen
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Jul 22, 2019·The Journal of Chemical Physics·Gaia CamisascaLars G M Pettersson
Jun 17, 2019·The Journal of Chemical Physics·Gaia CamisascaLars G M Pettersson
Aug 29, 2020·Physical Review Letters·Kyung Hwan KimFivos Perakis
Sep 7, 2019·Physical Review Letters·Alfonso M Gañán-Calvo
Nov 5, 2020·Journal of Synchrotron Radiation·Nelson HuaOleg G Shpyrko
Feb 11, 2021·Journal of Synchrotron Radiation·Yanwen SunDiling Zhu
Oct 16, 2019·Langmuir : the ACS Journal of Surfaces and Colloids·Henning WeissMarkus Mezger
Oct 19, 2021·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Jie HuangShiben Li
Nov 12, 2021·The Journal of Physical Chemistry. B·Jakob PetersenRossend Rey

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Methods Mentioned

BETA
X-ray

Software Mentioned

XSVS
TIP4P
MB
pol
Gromacs

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