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Title: Structural, electronic, and dynamical properties of liquid water by ab initio molecular dynamics based on SCAN functional within the canonical ensemble

Abstract

We perform ab initio molecular dynamics (AIMD) simulation of liquid water in the canonical ensemble at ambient conditions using the strongly constrained and appropriately normed (SCAN) meta-generalized-gradient approximation (GGA) functional approximation and carry out systematic comparisons with the results obtained from the GGA-level Perdew-Burke-Ernzerhof (PBE) functional and Tkatchenko-Scheffler van der Waals (vdW) dispersion correction inclusive PBE functional. We analyze various properties of liquid water including radial distribution functions, oxygen-oxygen-oxygen triplet angular distribution, tetrahedrality, hydrogen bonds, diffusion coefficients, ring statistics, density of states, band gaps, and dipole moments. We find that the SCAN functional is generally more accurate than the other two functionals for liquid water by not only capturing the intermediate-range vdW interactions but also mitigating the overly strong hydrogen bonds prescribed in PBE simulations. We also compare the results of SCAN-based AIMD simulations in the canonical and isothermal-isobaric ensembles. Our results suggest that SCAN provides a reliable description for most structural, electronic, and dynamical properties in liquid water.

Authors:
ORCiD logo [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [3];  [1];  [4]
  1. Temple Univ., Philadelphia, PA (United States). Dept. of Physics
  2. Department of Chemistry, Princeton University, Princeton, New Jersey 08544, USA
  3. Princeton Univ., NJ (United States). Dept. of Chemistry
  4. Temple Univ., Philadelphia, PA (United States). Dept. of Physics, and Inst. for Computational Molecular Science
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for the Computational Design of Functional Layered Materials (CCDM)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF); American Chemical Society (ACS)
OSTI Identifier:
1470566
Alternate Identifier(s):
OSTI ID: 1435002
Grant/Contract Number:  
SC0012575; AC02-05CH11231; 53482-DNI6
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 148; Journal Issue: 16; Related Information: CCDM partners with Temple University (lead); Brookhaven National Laboratory; Drexel University; Duke University; North Carolina State University; Northeastern University; Princeton University; Rice University; University of Pennsylvania; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; catalysis (heterogeneous); solar (photovoltaic); energy storage (including batteries and capacitors); hydrogen and fuel cells; defects; mechanical behavior; materials and chemistry by design; synthesis (novel materials)

Citation Formats

Zheng, Lixin, Chen, Mohan, Sun, Zhaoru, Ko, Hsin-Yu, Santra, Biswajit, Dhuvad, Pratikkumar, and Wu, Xifan. Structural, electronic, and dynamical properties of liquid water by ab initio molecular dynamics based on SCAN functional within the canonical ensemble. United States: N. p., 2018. Web. doi:10.1063/1.5023611.
Zheng, Lixin, Chen, Mohan, Sun, Zhaoru, Ko, Hsin-Yu, Santra, Biswajit, Dhuvad, Pratikkumar, & Wu, Xifan. Structural, electronic, and dynamical properties of liquid water by ab initio molecular dynamics based on SCAN functional within the canonical ensemble. United States. doi:10.1063/1.5023611.
Zheng, Lixin, Chen, Mohan, Sun, Zhaoru, Ko, Hsin-Yu, Santra, Biswajit, Dhuvad, Pratikkumar, and Wu, Xifan. Fri . "Structural, electronic, and dynamical properties of liquid water by ab initio molecular dynamics based on SCAN functional within the canonical ensemble". United States. doi:10.1063/1.5023611. https://www.osti.gov/servlets/purl/1470566.
@article{osti_1470566,
title = {Structural, electronic, and dynamical properties of liquid water by ab initio molecular dynamics based on SCAN functional within the canonical ensemble},
author = {Zheng, Lixin and Chen, Mohan and Sun, Zhaoru and Ko, Hsin-Yu and Santra, Biswajit and Dhuvad, Pratikkumar and Wu, Xifan},
abstractNote = {We perform ab initio molecular dynamics (AIMD) simulation of liquid water in the canonical ensemble at ambient conditions using the strongly constrained and appropriately normed (SCAN) meta-generalized-gradient approximation (GGA) functional approximation and carry out systematic comparisons with the results obtained from the GGA-level Perdew-Burke-Ernzerhof (PBE) functional and Tkatchenko-Scheffler van der Waals (vdW) dispersion correction inclusive PBE functional. We analyze various properties of liquid water including radial distribution functions, oxygen-oxygen-oxygen triplet angular distribution, tetrahedrality, hydrogen bonds, diffusion coefficients, ring statistics, density of states, band gaps, and dipole moments. We find that the SCAN functional is generally more accurate than the other two functionals for liquid water by not only capturing the intermediate-range vdW interactions but also mitigating the overly strong hydrogen bonds prescribed in PBE simulations. We also compare the results of SCAN-based AIMD simulations in the canonical and isothermal-isobaric ensembles. Our results suggest that SCAN provides a reliable description for most structural, electronic, and dynamical properties in liquid water.},
doi = {10.1063/1.5023611},
journal = {Journal of Chemical Physics},
number = 16,
volume = 148,
place = {United States},
year = {2018},
month = {4}
}

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