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Lorenz, Marco ; Maschio, Lorenzo ; Usvyat, Denis ; Schütz, Martin

Local ab initio methods for calculating optical bandgaps in periodic systems. II. Periodic density fitted local configuration interaction singles method for solids

Lorenz, Marco, Maschio, Lorenzo , Usvyat, Denis and Schütz, Martin (2012) Local ab initio methods for calculating optical bandgaps in periodic systems. II. Periodic density fitted local configuration interaction singles method for solids. Journal of Chemical Physics 137, p. 204119.

Date of publication of this fulltext: 24 Oct 2016 14:12
Article
DOI to cite this document: 10.5283/epub.34754


Abstract

We present a density fitted local configuration interaction singles (CIS) method for calculating optical bandgaps in 3D-periodic systems. We employ an Ewald technique to carry out infinite lattice summations for the exciton-exciton interaction, and robust product-density specific local density fitting in direct space for the electron-hole interaction. Moreover, we propose an alternative to the ...

We present a density fitted local configuration interaction singles (CIS) method for calculating optical bandgaps in 3D-periodic systems. We employ an Ewald technique to carry out infinite lattice summations for the exciton-exciton interaction, and robust product-density specific local density fitting in direct space for the electron-hole interaction. Moreover, we propose an alternative to the usual cyclic model with Born-von Karman periodic boundary conditions, the so called Wigner-Seitz supercell truncated infinite model, which exhibits much improved convergence of the CIS excitation energy with respect to the size of the supercell. Test calculations on a series of prototypical systems demonstrate that the method at the present stage can be used to calculate the excitonic bandgaps of 3D periodic systems with up to a dozen atoms in the unit cell, ranging from wide-gap insulators to semiconductors. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4767775]



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Details

Item typeArticle
Journal or Publication TitleJournal of Chemical Physics
Publisher:AMER INST PHYSICS
Open Access Type:Alliance-/National licence
Place of Publication:MELVILLE
Volume:137
Page Range:p. 204119
Date2012
InstitutionsChemistry and Pharmacy > Institut für Physikalische und Theoretische Chemie > Research Group Theoretical Chemistry > Prof. Dr. Martin Schütz
Chemistry and Pharmacy > Institut für Physikalische und Theoretische Chemie > Research Group Theoretical Chemistry > PD Dr. Denis Usvyat
Identification Number
ValueType
10.1063/1.4767775DOI
KeywordsELECTRONIC EXCITED-STATES; GAUSSIAN-BASIS SETS; HARTREE-FOCK; EXTENDED SYSTEMS; LINEAR-COMBINATION; FUNCTIONAL THEORY; WANNIER FUNCTIONS; COUPLED-CLUSTER; GREENS-FUNCTION; COULOMB PROBLEM;
Dewey Decimal Classification500 Science > 540 Chemistry & allied sciences
StatusPublished
RefereedYes, this version has been refereed
Created at the University of RegensburgYes
URN of the UB Regensburgurn:nbn:de:bvb:355-epub-347544
Item ID34754

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