Lorenz, Marco and Usvyat, Denis and Schuetz, Martin (2011) Local ab initio methods for calculating optical band gaps in periodic systems. I. Periodic density fitted local configuration interaction singles method for polymers. JOURNAL OF CHEMICAL PHYSICS, 134 (9): 094101. ISSN 0021-9606,
Full text not available from this repository. (Request a copy)Abstract
We present a density fitted local configuration interaction singles (CIS) method for calculating optical band gaps in 1D-periodic systems. The method is based on the Davidson diagonalization procedure, carried out in the reciprocal space. The one-electron part of the matrix-vector products is also evaluated in the reciprocal space, where the diagonality of the Fock matrix can be exploited. The contraction of the CIS vectors with the two electron integrals is performed in the direct space in the basis of localized occupied (Wannier) and virtual (projected atomic) orbitals. The direct space approach allows to utilize the sparsity of the integrals due to the local representation and locality of the exciton. The density fitting approximation employed for the two electron integrals reduces the nominal scaling with unit cell size to O(N(4)). Test calculations on a series of prototypical systems demonstrate that the method in its present stage can be used to calculate the excitonic band gaps of polymers with up to a few dozens of atoms in the cell. The computational cost depends on the locality of the exciton, but even relatively delocalized excitons occurring in the polybiphenyl in the parallel orientation, can be routinely treated with this method. (C) 2011 American Institute of Physics. [doi: 10.1063/1.3554209]
| Item Type: | Article |
|---|---|
| Uncontrolled Keywords: | ELECTRONIC EXCITED-STATES; PLESSET PERTURBATION-THEORY; COMPOSITE ENERGY-BANDS; WANNIER FUNCTIONS; HARTREE-FOCK; EXTENDED SYSTEMS; COUPLED-CLUSTER; GREENS-FUNCTION; LINEAR-COMBINATION; FUNCTIONAL THEORY; |
| Subjects: | 500 Science > 540 Chemistry & allied sciences |
| Divisions: | Chemistry 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 |
| Depositing User: | Dr. Gernot Deinzer |
| Date Deposited: | 24 Jun 2020 05:52 |
| Last Modified: | 24 Jun 2020 05:52 |
| URI: | https://pred.uni-regensburg.de/id/eprint/21121 |
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