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Light-induced nonadiabatic energy- and charge transfer dynamics

光诱导的非绝热能量和电荷转移动力学

基本信息

批准号：
278151256
负责人：
Professor Dr. Roland Mitric
金额：
--
依托单位：
Institut für Physikalische und Theoretische Chemie
依托单位国家：
德国
项目类别：
Research Units
财政年份：
2015
资助国家：
德国
起止时间：
2014-12-31 至 2018-12-31
项目状态：
已结题

来源：
https://gepris.dfg.de/gepris/projekt/278151256?language=en
关键词：
Light induced nonadiabatic energy charge

项目摘要

The aim of the present project is the development of an efficient mixed quantum-classical methodology for the simulation of light-induced nonadiabatic dynamical processes in multichromophoric molecular aggregates. The dynamics of energy and charge transfer in such systems represents a hot topic of the state-of-the-art experimental research The energy and charge transfer dynamics in these systems is a hot topic of the state-of-the-art experimental research and there is growing evidence that nonadiabatic radiationless relaxation processes play a fundamental role in determining the efficiency of the exciton transfer or charge transport. In addition to the intramolecular nonradiative transitions through conical intersections, which play a fundamental role in photochemistry and photophysics, the coupling between the individual chromophores in multichromophoric assemblies gives rise to novel intermolecular nonradiative relaxation channels through funnels between the delocalized excitonic and/or charge transfer states. To simulate the energy and charge transfer dynamics in multichromophoric nanostructures we will develop and implement a combined methodology of light-induced surface hopping methods and efficient electronic structure calculations based on the long-range corrected time-dependent density functional tight-binding method. In order to directly compare our theoretical results with experimental findings and to support the interpretation of the latter, we will supplement our method by developing a theoretical approach for the simulation of time-resolved multidimensional spectra. This methodology will be applied for the simulation of the conformational dynamics and light-induced dynamical processes of squaraine oligomers in different solvent environments.

本项目的目的是发展一种有效的混合量子-经典方法，用于模拟多色分子聚集体中的光诱导非绝热动力学过程。这些系统中的能量和电荷转移动力学是最先进的实验研究的一个热门话题。这些系统中的能量和电荷转移动力学是最先进的实验研究的一个热门话题，并且越来越多的证据表明，非绝热无辐射弛豫过程在确定激子转移或电荷输运的效率中起着根本性的作用。除了通过圆锥形交叉点的分子内非辐射跃迁，这在光化学和光物理学中起着重要作用，在多发色团组装中的各个发色团之间的耦合通过离域激子和/或电荷转移状态之间的漏斗产生了新的分子间非辐射弛豫通道。为了模拟多发色团纳米结构中的能量和电荷转移动力学，我们将开发和实施基于长程校正的时间依赖密度泛函紧束缚方法的光诱导表面跳跃方法和有效的电子结构计算的组合方法。为了直接比较我们的理论结果与实验结果，并支持后者的解释，我们将补充我们的方法，通过开发一个理论方法的时间分辨多维光谱的模拟。这种方法将被应用于模拟的构象动力学和光诱导的动力学过程的方酸寡聚体在不同的溶剂环境。