Influence of the exchange-correlation functional on the quasi-harmonic lattice dynamics of II-VI semiconductors
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Published version
Author(s)
Type
Journal Article
Abstract
We perform a systematic comparison of the finite-temperature structure and properties of four bulk semiconductors (PbS, PbTe, ZnS, and ZnTe) predicted by eight popular exchange-correlation functionals from quasi-harmonic lattice-dynamics calculations. The performance of the functionals in reproducing the temperature dependence of a number of material properties, including lattice parameters, thermal-expansion coefficients, bulk moduli, heat capacities, and phonon frequencies, is evaluated quantitatively against available experimental data. We find that the phenomenological over- and under-binding characteristics of the local-density approximation and the PW91 and Perdew-Burke-Enzerhof (PBE) generalised-gradient approximation (GGA) functionals, respectively, are exaggerated at finite temperature, whereas the PBEsol GGA shows good general performance across all four systems. The Tao-Perdew-Staroverov-Scuseria (TPSS) and revTPSS meta-GGAs provide relatively small improvements over PBE, with the latter being better suited to calculating structural and dynamical properties, but both are considerably more computationally demanding than the simpler GGAs. The dispersion-corrected PBE-D2 and PBE-D3 functionals perform well in describing the lattice dynamics of the zinc chalcogenides, whereas the lead chalcogenides appear to be challenging for these functionals. These findings show that quasi-harmonic calculations with a suitable functional can predict finite-temperature structure and properties with useful accuracy, and that this technique can serve as a means of evaluating the performance of new functionals in the future.
Date Issued
2015-08-14
Date Acceptance
2015-07-23
Citation
Journal of Chemical Physics, 2015, 143 (6)
ISSN
1089-7690
Publisher
AIP Publishing
Journal / Book Title
Journal of Chemical Physics
Volume
143
Issue
6
Copyright Statement
© 2015 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution 3.0 Unported License (https://creativecommons.org/licenses/by/3.0/).
Identifier
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000359799600041&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
Subjects
Science & Technology
Physical Sciences
Chemistry, Physical
Physics, Atomic, Molecular & Chemical
Chemistry
Physics
GENERALIZED-GRADIENT APPROXIMATION
AUGMENTED-WAVE METHOD
ELASTIC-CONSTANTS
THERMAL-EXPANSION
LOCAL-DENSITY
ALL-ELECTRON
ULTRASOFT PSEUDOPOTENTIALS
THERMOELASTIC PROPERTIES
NONPRIMITIVE LATTICES
STRUCTURAL-PROPERTIES
Chemical Physics
02 Physical Sciences
03 Chemical Sciences
09 Engineering
Publication Status
Published
Article Number
ARTN 064710