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Hier finden Sie wissenschaftliche Publikationen aus den FraunhoferInstituten. Accuracy of Hybrid Functionals with NonSelfConsistent KohnSham Orbitals for Predicting the Properties of Semiconductors
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Skelton, J.M.; Gunn, D.S.D.; Metz, S.; Parker, S.C.  Journal of chemical theory and computation : JCTC 16 (2020), Nr.6, S.35433557 ISSN: 15499618 ISSN: 15499626 

 Englisch 
 Zeitschriftenaufsatz 
 Fraunhofer ISE () 
Abstract
Accurately modeling the electronic structure of materials is a persistent challenge to highthroughput screening. A promising means of balancing accuracy against computational cost is nonselfconsistent calculations with hybrid densityfunctional theory, where the electronic band energies are evaluated using a hybrid functional from orbitals obtained with a less demanding (semi)local functional. We have quantified the performance of this technique for predicting the physical properties of 16 tetrahedral semiconductors with bandgaps from 0.2 to 5.5 eV. Provided the base functional predicts a nonmetallic electronic structure, bandgaps within 5% of the PBE0 and HSE06 gaps can be obtained with an order of magnitude reduction in computing time. The positions of the valence and conduction band extrema and the Fermi level are well reproduced, enabling calculation of the band dispersion, density of states, and dielectric properties using Fermi’s Golden Rule. While the error in the nonselfconsistent total energies is ∼50 meV atom–1, the energyvolume curves are reproduced accurately enough to obtain the equilibrium volume and bulk modulus with minimal error. We also test the dielectricdependent scPBE0 functional and obtain bandgaps and dielectric constants to within 2.5% of the selfconsistent results, which amounts to a significant improvement over selfconsistent PBE0 for a similar computational cost. We identify cases where the nonselfconsistent approach is expected to perform poorly and demonstrate that partial selfconsistency provides a practical and efficient workaround. Finally, we perform proofofconcept calculations on CoO and NiO to demonstrate the applicability of the technique to strongly correlated openshell transitionmetal oxides.