Photophysics of organic photostabilizers: ab initio electronic-structure and quantum-dynamics calculations

有机光稳定剂的光物理学：从头算电子结构和量子动力学计算

• 批准号: 32931736
• 负责人: Professor Dr. Wolfgang Domcke
• 金额: --
• 依托单位: Lehrstuhl für Theoretische Chemie
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2006
• 资助国家: 德国
• 起止时间: 2005-12-31 至 2010-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/32931736?language=en
• 关键词: Photophysics; organic; photostabilizers; ab; initio

The aim of this project is the investigation of the dynamical processes which account for the functionality of organic photostabilizers, using the tools of computational chemistry. Ab initio electronic-structure theory will be employed to determine the essential features of the excited-state and ground-state potential-energy surfaces. A primary goal is the identification and characterization of conical intersections of the energy surfaces of the lowest exited singlet state (S1) and the electronic ground state (S0). These conical intersections serve as photochemical funnels for the ultrafast deactivation of the excited state. The dynamics of the S1¿S0 radiationless decay processes at the S1-S0 conical intersections will be investigated with time-dependent quantum wave-packet methods. The theoretical studies will be focused on three intramolecularly hydrogen-bonded aromatic systems for which an extensive set of experimental data is available: ohydroxybenzaldehyde, salicylic acid and 2-(2 -hydroxyphenyl)benzotriazole (TINUVIN). Summary of the interaction: The ab initio electronic-structure calculations will be performed in the group of A. L. Sobolewski in Warsaw. This includes the exploration of exited-state potential-energy surfaces, the determination of reaction paths and conical intersections, as well as the calculation of ab initio energy data on large grids in nuclear coordinate space. Multidimensional multi-sheeted analytic potential-energy functions will be constructed in the group of W. Domcke in Munich, using the ab initio-data provided by the Warsaw group. The time-dependent quantum reaction dynamics computations will be performed with the programs available in the Munich group. Much of the exchange of information will occur by email or file transfer. To broaden the education of the students and/or postdocs, these coworkers will visit the respective partner group once per year.

本项目的目的是利用计算化学的工具来研究有机光稳定剂的功能性的动力学过程。从头算电子结构理论将被用来确定激发态和基态势能面的基本特征。一个主要目标是最低激发单重态（S1）和电子基态（S 0）的能量表面的锥形交叉点的识别和表征。这些锥形交叉点作为光化学漏斗，用于激发态的超快失活。S1的动力学？用含时量子波包方法研究了S_1-S_0锥交点处的S_0无辐射衰变过程。理论研究将集中在三个分子内氢键的芳香族系统，其中一组广泛的实验数据是可用的：邻羟基苯甲醛，水杨酸和2-（2 -羟基苯基）苯并三唑（TINUVIN）。相互作用总结：将在A组中进行从头计算电子结构计算。L.华沙的索博列夫斯基。这包括探索激发态势能面，确定反应路径和圆锥交点，以及在核坐标空间中的大网格上计算从头算能量数据。在W群中构造多维多层解析势能函数。Domcke在慕尼黑，使用华沙小组提供的从头算数据。含时量子反应动力学计算将使用慕尼黑小组提供的程序进行。大部分信息交换将通过电子邮件或文件传输进行。为了扩大学生和/或博士后的教育，这些同事将每年访问各自的合作伙伴团体一次。