Title

Comparison of real-time and linear-response time-dependent density functional theories for molecular chromophores ranging from sparse to high densities of states

Document Type

Article

Publication Date

3-10-2015

Abstract

© 2015 American Chemical Society. We assess the performance of real-time time-dependent density functional theory (RT-TDDFT) for the calculation of absorption spectra of 12 organic dye molecules relevant to photovoltaics and dye-sensitized solar cells with 8 exchange-correlation functionals (3 traditional, 3 global hybrids, and 2 range-separated hybrids). We compare the calculations with traditional linear-response (LR) TDDFT and experimental spectra. In addition, we demonstrate the efficacy of the RT-TDDFT approach to calculate wide absorption spectra of two large chromophores relevant to photovoltaics and molecular switches. RT-TDDFT generally requires longer simulation times, compared to LR-TDDFT, for absorption spectra of small systems. However, it becomes more effective for the calculation of wide absorption spectra of large molecular complexes and systems with very high densities of states.

Publication Source (Journal or Book title)

Journal of Chemical Theory and Computation

First Page

1102

Last Page

1109

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