X-Ray Absorption Signatures of the Molecular Environment in Water and Ice

被引：83

作者：

Chen, Wei ^{[1
]}

Wu, Xifan ^{[2
]}

Car, Roberto ^{[1
,2
,3
]}

机构：

[1] Princeton Univ, Dept Phys, Princeton, NJ 08544 USA

[2] Princeton Univ, Dept Chem, Princeton, NJ 08544 USA

[3] Princeton Univ, Princeton Inst Sci & Technol Mat, Princeton, NJ 08544 USA

来源：

PHYSICAL REVIEW LETTERS | 2010年 / 105卷 / 01期

基金：

美国国家科学基金会;

关键词：

HYDROGEN-BOND NETWORK; FINAL-STATE RULE; LIQUID WATER; SPECTRA; REARRANGEMENTS; ENERGETICS; DYNAMICS;

D O I：

10.1103/PhysRevLett.105.017802

中图分类号：

O4 [物理学];

学科分类号：

0702 ;

摘要：

The x-ray absorption spectra of water and ice are calculated with a many-body approach for electron-hole excitations. The experimental features, including the effects of temperature change in the liquid, are reproduced from configurations generated by ab initio molecular dynamics. The spectral difference between the solid and the liquid is due to two major short-range order effects. One, due to breaking of hydrogen bonds, enhances the pre-edge intensity in the liquid. The other, due to a nonbonded molecular fraction in the first coordination shell, affects the main spectral edge in the conversion of ice to water. This effect may not involve hydrogen bond breaking as shown by experiment in high-density amorphous ice.

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