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Issue 2, 2010
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Reformulating time-dependent density functional theory with non-orthogonal localized molecular orbitals

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Abstract

Time-dependent density functional theory (TDDFT) has broad application in the study of electronic response, excitation and transport. To extend such application to large and complex systems, we develop a reformulation of TDDFT equations in terms of non-orthogonal localized molecular orbitals (NOLMOs). NOLMO is the most localized representation of electronic degrees of freedom and has been used in ground state calculations. In atomic orbital (AO) representation, the sparsity of NOLMO is transferred to the coefficient matrix of molecular orbitals (MOs). Its novel use in TDDFT here leads to a very simple form of time propagation equations which can be solved with linear-scaling effort. We have tested the method for several long-chain saturated and conjugated molecular systems within the self-consistent charge density-functional tight-binding method (SCC-DFTB) and demonstrated its accuracy. This opens up pathways for TDDFT applications to large bio- and nano- systems.

Graphical abstract: Reformulating time-dependent density functional theory with non-orthogonal localized molecular orbitals

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Publication details

The article was received on 12 Aug 2009, accepted on 19 Oct 2009 and first published on 13 Nov 2009


Article type: Paper
DOI: 10.1039/B916688B
Citation: Phys. Chem. Chem. Phys., 2010,12, 416-421
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    Reformulating time-dependent density functional theory with non-orthogonal localized molecular orbitals

    G. Cui, W. Fang and W. Yang, Phys. Chem. Chem. Phys., 2010, 12, 416
    DOI: 10.1039/B916688B

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