Dipartimento di Chimica e Chimica Industriale, University of Pisa, via Moruzzi 13, 56124 Pisa, Italy.
J Chem Theory Comput. 2021 Dec 14;17(12):7373-7383. doi: 10.1021/acs.jctc.1c00942. Epub 2021 Nov 29.
We present an implementation of the Frenkel exciton model in the framework of the semiempirical floating occupation molecular orbitals-configuration interaction (FOMO-CI) electronic structure method, aimed at simulating the dynamics of multichromophoric systems, in which excitation energy transfer can occur, by a very efficient approach. The nonadiabatic molecular dynamics is here dealt with by the surface hopping method, but the implementation we proposed is compatible with other dynamical approaches. The exciton coupling is computed either exactly, within the semiempirical approximation considered, or by resorting to transition atomic charges. The validation of our implementation is carried out on the -azobenzeno-2S-phane (2S-TTABP), formed by two azobenzene units held together by sulfur bridges, taken as a minimal model of multichromophoric systems, in which both strong and weak exciton couplings are present.
我们提出了在半经验浮置占据分子轨道-组态相互作用（FOMO-CI）电子结构方法的框架内实现弗伦克尔激子模型，旨在通过非常有效的方法模拟多发色团体系的动力学，其中可能发生激发能量转移。非绝热分子动力学通过表面跳跃方法来处理，但我们提出的实现方式与其他动力学方法兼容。激子耦合可以在半经验近似中进行精确计算，也可以通过过渡原子电荷来计算。我们的实现的验证是在-偶氮苯-2S-螺环（2S-TTABP）上进行的，它由两个通过硫桥连接的偶氮苯单元组成，作为多发色团体系的最小模型，其中存在强和弱激子耦合。
