分子激发态动力学研究立项报告

摘 要：發生在激发态的光解离、异构化、光致电子或质子转移等化学反应过程，以及激发态分子间的能量传递、转换等动力学过程在能源、大气化学以及生物学等领域都至关重要。针对激发态分子反应动力学的研究，该研究将聚焦在以下几方面研究：（1）利用飞秒泵浦-探测技术等时间分辨光谱技术研究光化学、太阳能转化材料和生物分子检测中重要体系的激发态动力学过程；（2）利用单分子光谱技术研究单个超支化分子单光子发射的特点以及分子内各个分支之间的强或弱相干耦合作用的机理和规律；（3）利用实验方法，研究复杂体系中如化学激光体系，大气化学体系中重要激发态原子分子的传能以及非绝热反应动力学；（4）利用各种先进的实验方法，研究复杂体系光解离过程的非绝热动力学，特别是电子激发态与基态之间，以及激发态与激发态之间的锥形交叉点非绝热动力学的研究；（5）发展新的能够计算凝聚态复杂分子体系非绝热过程的动力学理论方法，并利用动力学理论方法来阐述复杂分子体系的激发态动力学机理。通过该研究，我们将在“分子激发态动力学”这个前沿性科学问题研究上取得突破性进展，取得一批具有重要影响力的创新性研究结果。

关键词：分子激发态 反应动力学 时间分辨光谱 光解离 复杂分子体系

The Project Report of the Study of Excited Molecular Dynamics

Han Keli1 Yang Heping1 Mo Yuxiang2 Xia Andong3 Yuan Kaijun1

（1.Dalian Institute of Chemical Physics，Chinese Academy of Sciences； 2.Tsinghua University；

3.Institute of Chemistry， Chinese Academy of Sciences）

Abstract：The chemical reactions which happened on the excited states， such as photolysis， isomerization， photo induced electron or proton transfer， and the dynamic process of energy transfer and conversion between excited molecules are very important in the study area of energy，atmospheric chemistry and biology. In this project， we will study the following aspects in the area of excited molecular dynamics. （1）We will use the time-resolved spectroscopy， such as the femtosecond pump-probe method， to study the excited molecular dynamics of important molecules in photochemistry， solar energy conversion material and biologic molecular detection. （2）The single molecule spectroscopy will be used to study the single photo emission of single hyper-branched molecules and the mechanism of strong or weak coupling between branches. （3）To study the energy transfer and nonadiabatic reaction dynamics of excited atoms and molecules in complex systems， such as chemical laser and atmospheric chemistry systems， by experiments. （4）Using the advanced experiment techniques to study the nonadiabatic dynamics in photolysis reactions， especially the nonadiabatic dynamics on the cone crossing point between electronic excited states， or between the excited states and ground states. （5）Developing new dynamic theory to study the nonadiabatic process of complex molecular systems in condensed states， and using this new theory to explain the dynamics of complex molecules on excited states. By the work of this project， we will get some innovated results， and make some important processes in the study of the excited molecular dynamics.

Key Words：Excited states； Reaction dynamics； Time-resolved spectroscopy； Photolysis； Complex molecular system