Fast construction of the Kohn-Sham response function for molecules

被引：8

作者：

Koval, Peter ^{[1
]}

Foerster, Dietrich ^{[2
]}

Coulaud, Olivier ^{[3
]}

机构：

[1] INRIA Sud Ouest, HiePACS Project, CNRS, F-33405 Talence, France

[2] Univ Bordeaux 1, CPMOH, F-33405 Talence, France

[3] INRIA Bordeaux Sud Ouest, HiePACS Project, F-33405 Talence, France

来源：

PHYSICA STATUS SOLIDI B-BASIC SOLID STATE PHYSICS | 2010年 / 247卷 / 08期

关键词：

density functional theory; Kohn-Sham response; LCAO basis set; molecules; molecular spectra; CHOLESKY DECOMPOSITIONS; EXCITATION-ENERGIES; BASIS-SETS; ABSORPTION;

D O I：

10.1002/pssb.200983811

中图分类号：

O469 [凝聚态物理学];

学科分类号：

070205 ;

摘要：

The use of the linear combination of atomic orbitals method for excited states involves products of orbitals that are known to be linearly dependent. We identify a basis in the space of orbital products that is local for orbitals of finite support and with a residual error that vanishes exponentially with its dimension. As an application of our previously reported technique we compute the Kohn-Sham density response function chi(0) for a molecule consisting of N atoms in (NN omega)-N-2, operations, with N-omega the number of frequency points. We test our construction of chi(0) by computing molecular spectra directly from the equations of Petersilka-Gossmann-Gross in (NN omega)-N-2 operations rather than from Casida's equations which takes N-3 operations. We consider the good agreement with previously calculated molecular spectra as a validation of our construction of chi(0). Ongoing work indicates that our method is well suited for the computation of the GW self-energy Sigma = iGW and we expect it to be useful in the analysis of exitonic effects in molecules. (C) 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

引用

页码：1841 / 1848

页数：8

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