期刊
JOURNAL OF CHEMICAL PHYSICS
卷 133, 期 11, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.3479401
关键词
ab initio calculations; density functional theory; electron correlations; exchange interactions (electron); excited states; polymers
资金
- Swedish National Infrastructure for Computing (SNIC) [SNIC 022/09-25]
We analyze the ability of spin-flip time dependent density functional theory (TD-DFT) to uniformly describe excited states of single, double, and mixed excitation character in closed-shell molecular systems, using the polyene oligomers as a primary test case. The results of comparison between conventional and spin-flip TD-DFT and with correlated ab initio methods indicate that spin-flip TD-DFT provides a more consistent description of the ordering and relative positions of the excited states than conventional TD-DFT provided a suitable exchange-correlation functional is used in the calculations. It is found that spin-flip TD-DFT provides a physically appealing picture of excitation processes which involve one or two electrons, as it captures their most important features and facilitates a more uniform description of excited states with different character. This makes spin-flip TD-DFT a promising approach for general modeling of excited states and spectra of medium and large size molecules, which exhibit low-lying excited states with strong double excitation character. (c) 2010 American Institute of Physics. [doi:10.1063/1.3479401]
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