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Linear-Scaling Time-Dependent Density Functional Theory Based on the Idea of "From Fragments to Molecule"
Wu, Fangqin; Liu, Wenjian1; Zhang, Yong; Li, Zhendong
2011-11-01
Source PublicationJOURNAL OF CHEMICAL THEORY AND COMPUTATION
ISSN1549-9618
Volume7Issue:11Pages:3643-3660
AbstractTo circumvent the cubic scaling and convergence difficulties encountered in the standard top-down localization of the global canonical molecular orbitals (CMOs), a bottom-up localization scheme is proposed based on the idea of "from fragments to molecule". That is, the global localized MOs (LMOs), both occupied and unoccupied, are to be synthesized from the primitive fragment LMOs (pFLMOs) obtained from subsystem calculations. They are orthonormal but are still well localized on the parent fragments of the pFLMOs and can hence be termed as "fragment LMOs" (FLMOs). This has been achieved by making use of two important factors. Physically, it is the transferability of the locality of the fragments that serves as the basis. Mathematically, it is the special block-diagonalization of the Kohn-Sham matrix that allows retention of the locality: The occupied-occupied and virtual-virtual diagonal blocks are only minimally modified when the occupied-virtual off-diagonal blocks are annihilated. Such a bottom-up localization scheme is applicable to systems composed of all kinds of chemical bonds. It is then shown that, by a simple prescreening of the particle-hole pairs, the FLMO-based time-dependent density functional theory (TDDFT) can achieve linear scaling with respect to the system size, with a very small prefactor. As a proof of principle, representative model systems are taken as examples to demonstrate the accuracy and efficiency of the algorithms. As both the orbital picture and integral number of electrons are retained, the FLMO-TDDFT offers a clear characterization of the nature of the excited states in line with chemical/physical intuition.
DOI10.1021/ct200225v
Indexed BySCI
Language英语
WOS IDWOS:000296597300021
PublisherAMER CHEMICAL SOC
Citation statistics
Cited Times:42[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.iccas.ac.cn/handle/121111/73092
Collection中国科学院化学研究所
Corresponding AuthorLiu, Wenjian
Affiliation1.Peking Univ, Beijing Natl Lab Mol Sci,Coll Chem & Mol Engn, Inst Theoret & Computat Chem, State Key Lab Rare Earth Mat Chem & Applicat, Beijing 100871, Peoples R China
2.Peking Univ, Ctr Computat Sci & Engn, Beijing 100871, Peoples R China
Recommended Citation
GB/T 7714
Wu, Fangqin,Liu, Wenjian,Zhang, Yong,et al. Linear-Scaling Time-Dependent Density Functional Theory Based on the Idea of "From Fragments to Molecule"[J]. JOURNAL OF CHEMICAL THEORY AND COMPUTATION,2011,7(11):3643-3660.
APA Wu, Fangqin,Liu, Wenjian,Zhang, Yong,&Li, Zhendong.(2011).Linear-Scaling Time-Dependent Density Functional Theory Based on the Idea of "From Fragments to Molecule".JOURNAL OF CHEMICAL THEORY AND COMPUTATION,7(11),3643-3660.
MLA Wu, Fangqin,et al."Linear-Scaling Time-Dependent Density Functional Theory Based on the Idea of "From Fragments to Molecule"".JOURNAL OF CHEMICAL THEORY AND COMPUTATION 7.11(2011):3643-3660.
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