Influence of the exchange-correlation functional on the quasi-harmonic lattice dynamics of II-VI semiconductors

dc.contributor.authorWalsh, Aron
dc.contributor.authorSkelton, Jonathan M.
dc.contributor.authorTiana, Davide
dc.contributor.authorParker, Stephen C.
dc.contributor.authorTogo, Atsushi
dc.contributor.authorTanaka, Isao
dc.contributor.funderEngineering and Physical Sciences Research Councilen
dc.date.accessioned2018-07-06T09:01:26Z
dc.date.available2018-07-06T09:01:26Z
dc.date.issued2015-08
dc.date.updated2018-07-03T11:13:37Z
dc.description.abstractWe 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.en
dc.description.statusPeer revieweden
dc.description.versionPublished Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.citationSkelton, J. M., Tiana, D., Parker, S. C., Togo, A., Tanaka, I. and Walsh, A. (2015) 'Influence of the exchange-correlation functional on the quasi-harmonic lattice dynamics of II-VI semiconductors', The Journal of Chemical Physics, 143(6), 064710 (14 pp.) doi: 10.1063/1.4928058en
dc.identifier.doi10.1063/1.4928058
dc.identifier.endpage064710-14en
dc.identifier.issn0021-9606
dc.identifier.journaltitleChemical Physicsen
dc.identifier.startpage064710-1en
dc.identifier.urihttps://hdl.handle.net/10468/6423
dc.identifier.volume143en
dc.language.isoenen
dc.publisherAmerican Institute of Physics (AIP)en
dc.relation.projectinfo:eu-repo/grantAgreement/RCUK/EPSRC/EP/K004956/1/GB/Applying Long-lived Metastable States with Switchable Functionality via Kinetic Control of Molecular Assembly - a Programme in Functional Materials/en
dc.relation.projectinfo:eu-repo/grantAgreement/RCUK/EPSRC/EP/L000202/1/GB/MATERIALS CHEMISTRY HIGH END COMPUTING CONSORTIUM/en
dc.relation.urihttps://aip.scitation.org/doi/abs/10.1063/1.4928058
dc.rights© 2015 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution 3.0 Unported License.en
dc.subjectGeneralized-gradient approximationen
dc.subjectAugmented-wave methoden
dc.subjectElastic-constantsen
dc.subjectThermal-expansionen
dc.subjectLocal-densityen
dc.subjectAll-electronen
dc.subjectUltrasoft pseudopotentialsen
dc.subjectThermoelastic propertiesen
dc.subjectNonprimitive latticesen
dc.subjectStructural-propertiesen
dc.titleInfluence of the exchange-correlation functional on the quasi-harmonic lattice dynamics of II-VI semiconductorsen
dc.typeArticle (peer-reviewed)en
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