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

被引：64

作者：

Perakis, Fivos ^{[1
,2
]}

Camisasca, Gaia ^{[1
]}

Lane, Thomas J. ^{[2
]}

Spah, Alexander ^{[1
]}

Wikfeldt, Kjartan Thor ^{[1
]}

Sellberg, Jonas A. ^{[3
]}

Lehmkuehler, Felix ^{[4
,5
]}

Pathak, Harshad ^{[1
]}

Kim, Kyung Hwan ^{[1
]}

Amann-Winkel, Katrin ^{[1
]}

Schreck, Simon ^{[1
]}

Song, Sanghoon ^{[2
]}

Sato, Takahiro ^{[2
]}

Sikorski, Marcin ^{[2
,6
]}

Eilert, Andre ^{[2
]}

McQueen, Trevor ^{[2
]}

Ogasawara, Hirohito ^{[2
]}

Nordlund, Dennis ^{[2
]}

Roseker, Wojciech ^{[4
]}

Koralek, Jake ^{[2
]}

Nelson, Silke ^{[2
]}

Hart, Philip ^{[2
]}

Alonso-Mori, Roberto ^{[2
]}

Feng, Yiping ^{[2
]}

Zhu, Diling ^{[2
]}

Robert, Aymeric ^{[2
]}

Gruebel, Gerhard ^{[4
,5
]}

Pettersson, Lars G. M. ^{[1
]}

Nilsson, Anders ^{[1
]}

机构：

[1] Stockholm Univ, AlbaNova Univ Ctr, Dept Phys, S-10691 Stockholm, Sweden

[2] SLAC Natl Accelerator Lab, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA

[3] KTH Royal Inst Technol, AlbaNova Univ Ctr, Dept Appl Phys, Biomed & Xray Phys, S-10691 Stockholm, Sweden

[4] Deutsch Elektronen Synchrotron DESY, Notkestr 85, D-22607 Hamburg, Germany

[5] Hamburg Ctr Ultrafast Imaging, Luruper Chaussee 149, D-22761 Hamburg, Germany

[6] European XFEL, Holzkoppel 4, D-22869 Schenefeld, Germany

来源：

NATURE COMMUNICATIONS | 2018年 / 9卷

基金：

瑞典研究理事会; 欧洲研究理事会; 瑞士国家科学基金会;

关键词：

FREE-ELECTRON LASER; SPECKLE-VISIBILITY SPECTROSCOPY; PHOTON-CORRELATION SPECTROSCOPY; MOLECULAR-DYNAMICS; LIQUID WATER; TIME; SCATTERING; AMBIENT; DIFFRACTION; TIP4P/2005;

D O I：

10.1038/s41467-018-04330-5

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

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.

引用

页数：10

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