Fast Nonadiabatic Molecular Dynamics via Spin-Flip Time-Dependent Density-Functional Tight-Binding Approach: Application to Nonradiative Relaxation of Tetraphenylethylene with Locked Aromatic Rings

Hiroki Uratani, Toshiki Morioka, Takeshi Yoshikawa, Hiromi Nakai*

*この研究の対応する著者

研究成果: Article査読

3 被引用数 (Scopus)

抄録

Nonadiabatic dynamics around conical intersections between ground and excited states are crucial to understand excited-state phenomena in complex chemical systems. With this background in mind, we present an approach combining fewest-switches trajectory surface hopping and spin-flip (SF) time-dependent (TD) density-functional tight binding (DFTB), which is a simplified version of SF-TD density functional theory (DFT) with semiempirical parametrizations, for computationally efficient nonadiabatic molecular dynamics simulations. The estimated computational time of the SF-TD-DFTB approach is several orders of magnitude lower than that of SF-TD-DFT. In addition, the proposed method reproduces the time scales and quantum yields in photoisomerization reactions of azobenzene at a level comparable with conventional ab initio approaches, demonstrating reasonable accuracy. Finally, we report a practical application of the developed technique to explore the nonradiative relaxation processes of tetraphenylethylene and its derivative with torsionally locked aromatic rings and discuss the effect of locking the rings on the excited-state lifetime.

本文言語English
ページ(範囲)7299-7313
ページ数15
ジャーナルJournal of chemical theory and computation
16
12
DOI
出版ステータスPublished - 2020 12月 8

ASJC Scopus subject areas

  • コンピュータ サイエンスの応用
  • 物理化学および理論化学

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