Reformulating time-dependent density functional theory with non-orthogonal localized molecular orbitals.

Published

Journal Article

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.

Full Text

Duke Authors

Cited Authors

  • Cui, G; Fang, W; Yang, W

Published Date

  • January 2010

Published In

Volume / Issue

  • 12 / 2

Start / End Page

  • 416 - 421

PubMed ID

  • 20023819

Pubmed Central ID

  • 20023819

Electronic International Standard Serial Number (EISSN)

  • 1463-9084

International Standard Serial Number (ISSN)

  • 1463-9076

Digital Object Identifier (DOI)

  • 10.1039/b916688b

Language

  • eng