EXTRA-SHARC2 (Excited State Dynamics of Transition Metal Complexes using SHARC)

EXTRA-SHARC2（使用 SHARC 的过渡金属配合物的激发态动力学）

• 批准号: 403837698
• 负责人: Professorin Dr. Leticia González
• 金额: --
• 依托单位: Institut für Theoretische Chemie
• 依托单位国家: 德国
• 项目类别: Priority Programmes
• 资助国家: 德国
• 项目状态: 未结题
• 来源: https://gepris.dfg.de/gepris/projekt/403837698?language=en
• 关键词: EXTRA; SHARC2; Excited; State; Dynamics

The proposal EXTRA-SHARC2 is designed to continue our efforts in simulating the excited state dynamics of transition metal complexes investigated by synthetic and spectroscopic partners at the SPP2102. To this aim, we use our locally developed excited state molecular dynamics SHARC approach. SHARC stands for surface-hopping including arbitrary couplings and is able to describe internal conversion and intersystem crossing on the same footing. In the first funding period we employed SHARC combined with a linear vibronic coupling (LVC) model to parameterize the potential energy surfaces on which the nuclear dynamics is propagated, allowing for very efficient simulations of large complexes in full dimensionality. In the second funding period, this method (SHARC-LVC) is anticipated to be further employed and possibly extended in problematic cases. Effort will be put in dealing with molecules that possess an open-shell ground state, and involve doublet and quartet states. Our theoretical simulations are expected to deliver time-dependent deactivation mechanisms with atomistic resolution. In this way, this project will help rational design of novel Earth-abundant based photosensitizers and luminescent materials, as well as guide and predict strategies to control ligand dissociation or achieve directional electron transfer to be exploited in multiredox reactions.

EXTRA-SHARC 2提案旨在继续模拟SPP 2102的合成和光谱合作伙伴研究的过渡金属络合物的激发态动力学。为此，我们使用我们本地开发的激发态分子动力学SHARC方法。SHARC代表包括任意耦合的表面跳跃，并且能够在同一基础上描述内部转换和系统间交叉。在第一个资助期内，我们采用SHARC与线性振动耦合（LVC）模型相结合，以参数化核动力学传播的势能表面，从而可以非常有效地模拟全维度的大型复合物。在第二个供资期间，预计将进一步采用这种方法（SHARC-LVC），并可能在有问题的情况下延长。将努力处理具有开壳层基态的分子，并涉及二重态和四重态。我们的理论模拟有望提供原子级分辨率的时间依赖性失活机制。通过这种方式，该项目将有助于合理设计新型地球丰富的光敏剂和发光材料，以及指导和预测控制配体解离或实现多氧化还原反应中的定向电子转移的策略。