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Title: Communication: Dielectric properties of condensed systems composed of fragments

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.5044636· OSTI ID:1489283
ORCiD logo [1];  [2]; ORCiD logo [2]
  1. Hong Kong Univ. of Science and Technology, Hong Kong (China); HKUST Fok Ying Tung Research Institute, Guangzhou (China)
  2. Argonne National Lab. (ANL), Argonne, IL (United States); The Univ. of Chicago, Chicago, IL (United States)
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Here, the dielectric properties of molecules and nanostructures are usually modified in a complex manner, when assembled into a condensed phase. We propose a first-principles method to compute polarizabilities of sub-entities of solids and liquids, which accounts for multipolar interactions at all orders and is applicable to semiconductors and insulators. The method only requires the evaluation of induced fields in the condensed phase, with no need of multiple calculations for each constituent. As an example, we present results for the molecular polarizabilities of water in a wide pressure and temperature range. We found that at ambient conditions, the dipole-induced-dipole approximation is sufficiently accurate and the Clausius-Mossotti relation may be used, e.g., to obtain molecular polarizabilities from experimental refractive indexes. However with increasing pressure, this approximation becomes unreliable and in the case of ice X the Clausius-Mossotti relation is not valid.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
National Natural Science Foundation of China (NSFC); Alfred P. Sloan Foundation; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; Midwest Integrated Center for Computational Materials (MICCoM); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
Grant/Contract Number:
AC02-06CH11357; MICCoM
OSTI ID:
1489283
Alternate ID(s):
OSTI ID: 1462597
Journal Information:
Journal of Chemical Physics, Vol. 149, Issue 5; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 7 works
Citation information provided by
Web of Science

References (23)

Molecular polarizability of water from local dielectric response theory journal August 2017
First-Principles Approach to Insulators in Finite Electric Fields journal August 2002
Architecture of Qbox: A scalable first-principles molecular dynamics code journal January 2008
Wave-Number-Dependent Dielectric Function of Semiconductors journal December 1962
The Polarizability of Point-Polarizable Water Models:  Density Functional Theory/Molecular Mechanics Results † journal May 2008
Raman Spectra of Liquid Water from Ab Initio Molecular Dynamics: Vibrational Signatures of Charge Fluctuations in the Hydrogen Bond Network journal August 2013
van der Waals coefficient between closed shell ions journal January 1982
Dielectric properties of water under extreme conditions and transport of carbonates in the deep Earth journal March 2013
Perspective: Advances and challenges in treating van der Waals dispersion forces in density functional theory journal September 2012
Condensed phase ionic polarizabilities from plane wave density functional theory calculations journal October 2006
Local and Global Effects of Dissolved Sodium Chloride on the Structure of Water journal March 2017
Polarizabilities of individual molecules and ions in liquids from first principles journal November 2008
Microscopic local fields in dielectrics journal December 1979
The refractive index and electronic gap of water and ice increase with increasing pressure journal May 2014
Dielectric matrices and local fields in polar semiconductors journal June 1981
Anharmonic Raman Spectra in High-Pressure Ice from Ab Initio Simulations journal April 2002
Static compression of H2O-ice to 128 GPa (1.28 Mbar) journal December 1987
Equilibration and analysis of first-principles molecular dynamics simulations of water journal March 2018
Large variation of vacancy formation energies in the surface of crystalline ice journal September 2011
Large variation of vacancy formation energies in the surface of crystalline ice text January 2011
Maximally localized Wannier functions: Theory and applications text January 2011
The refractive index and electronic gap of water and ice increase with increasing pressure text January 2014
Molecular Polarizability of Water from the Local Dielectric Response Theory text January 2017

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36 MATERIALS SCIENCE