Wave-function-based approach to quasiparticle bands: Insight into the electronic structure of c-ZnS

A. Stoyanova, L. Hozoi, P. Fulde, and H. Stoll
Phys. Rev. B 83, 205119 – Published 19 May 2011

Abstract

Ab initio wave-function-based methods are employed for the study of quasiparticle energy bands of zinc-blende ZnS, with focus on the Zn 3d “semicore” states. The relative energies of these states with respect to the top of the S 3p valence bands appear to be poorly described as compared to experimental values not only within the local density approximation (LDA), but also when many-body corrections within the GW approximation are applied to the LDA or LDA + U mean-field solutions [T. Miyake, P. Zhang, M. L. Cohen, and S. G. Louie, Phys. Rev. B 74, 245213 (2006)]. In the present study, we show that for the accurate description of the Zn 3d states a correlation treatment based on wave-function methods is needed. Our study rests on a local Hamiltonian approach which rigorously describes the short-range polarization and charge redistribution effects around an extra hole or electron placed into the valence respective conduction bands of semiconductors and insulators. The method also facilitates the computation of electron correlation effects beyond relaxation and polarization. The electron correlation treatment is performed on finite clusters cut off the infinite system. The formalism makes use of localized Wannier functions and embedding potentials derived explicitly from prior periodic Hartree-Fock calculations. The on-site and nearest-neighbor charge relaxation lead to corrections of several eV to the Hartree-Fock band energies and gap. Corrections due to long-range polarization are of the order of 1.0 eV. The dispersion of the Hartree-Fock bands is only slightly affected by electron correlations. We find the Zn 3d “semicore” states to lie ~9.0 eV below the top of the S 3p valence bands, in very good agreement with values from valence-band x-ray photoemission.

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  • Received 15 December 2010

DOI:https://doi.org/10.1103/PhysRevB.83.205119

©2011 American Physical Society

Authors & Affiliations

A. Stoyanova1,2,*, L. Hozoi1,3, P. Fulde1,4, and H. Stoll5

  • 1Max-Planck-Institut für Physik komplexer Systeme, Nöthnitzer Strasse 38, D-01187 Dresden, Germany
  • 2Laboratoire de Chimie Quanitique, Institut de Chimie, CNRS/ Université de Strasbourg, 4 rue Blaise Pascal, F-6700 Strasbourg, France
  • 3Institut für Theoretische Festkörperphysik, Leibniz-Institut für Festkörper- und Werkstofforschung, Helmholtzstrasse 20, D-01069 Dresden, Germany
  • 4Asia Pacific Center for Theoretical Physics, Hogil Kim Memorial Building 501, POSTECH, San 31 Hyoja-dong, Namgu Pohang, Gyeongbuk 790-784, Korea
  • 5Institut für Theoretische Chemie, Universität Stuttgart, Pfaffenwaldring 55, D-70569 Stuttgart, Germany

  • *alex07@mpipks-dresden.mpg.de; stoyanova@unistra.fr

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Vol. 83, Iss. 20 — 15 May 2011

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