4.7 Article

Accurate Molecular Geometries in Complex Excited-State Potential Energy Surfaces from Time-Dependent Density Functional Theory

期刊

JOURNAL OF CHEMICAL THEORY AND COMPUTATION
卷 17, 期 1, 页码 357-366

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.jctc.0c00858

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资金

  1. Alexander von Humboldt Foundation
  2. Technical University of Munich-Institute for Advanced Study - German Excellence Initiative
  3. European Union Seventh Framework Programme [291763]
  4. Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) [EG397/4-1]

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In this study, it is suggested that using time-dependent density functional theory with optimally tuned range-separated hybrid functionals can accurately obtain excited-state molecular geometries, particularly in cases involving complex excited-state potential energy surfaces with local and charge-transfer excitations.
The interplay of electronic excitations and structural changes in molecules impacts nonradiative decay and charge transfer in the excited state, thus influencing excited-state lifetimes and photocatalytic reaction rates in optoelectronic and energy devices. To capture such effects requires computational methods providing an accurate description of excited-state potential energy surfaces and geometries. We suggest time-dependent density functional theory using optimally tuned range-separated hybrid (OT-RSH) functionals as an accurate approach to obtain excited-state molecular geometries. We show that OT-RSH provides accurate molecular geometries in excited-state potential energy surfaces that are complex and involve an interplay of local and charge-transfer excitations, for which conventional semilocal and hybrid functionals fail. At the same time, the nonempirical OT-RSH approach maintains the high accuracy of parametrized functionals (e.g., B3LYP) for predicting excited-state geometries of small organic molecules showing valence excited states.

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