Ab initio Electronic Structure of Liquid Water

被引：73

作者：

Chen, Wei ^{[1
]}

Ambrosio, Francesco ^{[1
]}

Miceli, Giacomo ^{[1
]}

Pasquarello, Alfredo ^{[1
]}

机构：

[1] Ecole Polytech Fed Lausanne, CSEA, CH-1015 Lausanne, Switzerland

来源：

PHYSICAL REVIEW LETTERS | 2016年 / 117卷 / 18期

基金：

瑞士国家科学基金会;

关键词：

DENSITY-FUNCTIONAL THEORY; CONDUCTION-BAND EDGE; ZERO-POINT MOTION; EMISSION-SPECTROSCOPY; DYNAMICS; PHOTOIONIZATION; PHOTOEMISSION; FLUCTUATIONS; SIMULATIONS; ISOTOPE;

D O I：

10.1103/PhysRevLett.117.186401

中图分类号：

O4 [物理学];

学科分类号：

0702 ;

摘要：

Self-consistent GW calculations with efficient vertex corrections are employed to determine the electronic structure of liquid water. Nuclear quantum effects are taken into account through ab initio path-integral molecular dynamics simulations. We reveal a sizable band-gap renormalization of up to 0.7 eV due to hydrogen-bond quantum fluctuations. Our calculations lead to a band gap of 8.9 eV, in accord with the experimental estimate. We further resolve the ambiguities in the band-edge positions of liquid water. The valence-band maximum and the conduction-band minimum are found at -9.4 and -0.5 eV with respect to the vacuum level, respectively.

引用

页数：6

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