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Title: First-principles study of the infrared spectrum in liquid water from a systematically improved description of H-bond network

Abstract

An accurate ab initio theory of the H-bond structure of liquid water requires a high-level exchange correlation approximation from density functional theory. Based on the liquid structures modeled by ab initio molecular dynamics by using maximally localized Wannier functions as a basis, we study the infrared spectrum of water within the canonical ensemble. In particular, we employ both the Perdew-Burke-Ernzerhof (PBE) functional within the generalized gradient approximation (GGA) and the state-of-the-art meta-GGA level approximation provided by the strongly constrained and appropriately normed (SCAN) functional. We demonstrate that the SCAN functional improves not only the water structure but also the theoretical infrared spectrum of water. Our analyses show that the improvement in the stretching and bending bands can be mainly attributed to better descriptions of directional H bonding and the covalency at the inter- and intramolecular levels, respectively. On the other hand, better agreements in libration and hindered translation bands are due to the improved dynamics of the H-bond network enabled by a less structured liquid in the experimental direction. The spectrum predicted by SCAN shows much better agreement with experimental data than the conventionally widely adopted PBE functional at the GGA level.

Authors:
 [1];  [2];  [3];  [4]
  1. Temple Univ., Philadelphia, PA (United States). Dept. of Physics
  2. Peking Univ., Beijing (China). College of Engineering, CAPT, HEDPS
  3. Chinese Academy of Sciences (CAS), Beijing (China). Inst. of Physics
  4. Temple Univ., Philadelphia, PA (United States). Dept. of Physics; Tample Univ., Philadelphia, PA (United States). Inst. for Computational Molecular Science
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Complex Materials from First Principles (CCM); Lawrence Berkeley National Laboratory-National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
OSTI Identifier:
1527149
DOE Contract Number:  
SC0012575; AC02-05CH11231
Resource Type:
Journal Article
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 99; Journal Issue: 20; Journal ID: ISSN 2469-9950
Country of Publication:
United States
Language:
English

Citation Formats

Xu, Jianhang, Chen, Mohan, Zhang, Cui, and Wu, Xifan. First-principles study of the infrared spectrum in liquid water from a systematically improved description of H-bond network. United States: N. p., 2019. Web. doi:10.1103/PhysRevB.99.205123.
Xu, Jianhang, Chen, Mohan, Zhang, Cui, & Wu, Xifan. First-principles study of the infrared spectrum in liquid water from a systematically improved description of H-bond network. United States. doi:10.1103/PhysRevB.99.205123.
Xu, Jianhang, Chen, Mohan, Zhang, Cui, and Wu, Xifan. Wed . "First-principles study of the infrared spectrum in liquid water from a systematically improved description of H-bond network". United States. doi:10.1103/PhysRevB.99.205123.
@article{osti_1527149,
title = {First-principles study of the infrared spectrum in liquid water from a systematically improved description of H-bond network},
author = {Xu, Jianhang and Chen, Mohan and Zhang, Cui and Wu, Xifan},
abstractNote = {An accurate ab initio theory of the H-bond structure of liquid water requires a high-level exchange correlation approximation from density functional theory. Based on the liquid structures modeled by ab initio molecular dynamics by using maximally localized Wannier functions as a basis, we study the infrared spectrum of water within the canonical ensemble. In particular, we employ both the Perdew-Burke-Ernzerhof (PBE) functional within the generalized gradient approximation (GGA) and the state-of-the-art meta-GGA level approximation provided by the strongly constrained and appropriately normed (SCAN) functional. We demonstrate that the SCAN functional improves not only the water structure but also the theoretical infrared spectrum of water. Our analyses show that the improvement in the stretching and bending bands can be mainly attributed to better descriptions of directional H bonding and the covalency at the inter- and intramolecular levels, respectively. On the other hand, better agreements in libration and hindered translation bands are due to the improved dynamics of the H-bond network enabled by a less structured liquid in the experimental direction. The spectrum predicted by SCAN shows much better agreement with experimental data than the conventionally widely adopted PBE functional at the GGA level.},
doi = {10.1103/PhysRevB.99.205123},
journal = {Physical Review B},
issn = {2469-9950},
number = 20,
volume = 99,
place = {United States},
year = {2019},
month = {5}
}

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