分子激發(fā)態(tài)動(dòng)力學(xué)研究立項(xiàng)報(bào)告

韓克利++楊何平++莫宇翔++夏安東++袁開軍

摘 要：發(fā)生在激發(fā)態(tài)的光解離、異構(gòu)化、光致電子或質(zhì)子轉(zhuǎn)移等化學(xué)反應(yīng)過程，以及激發(fā)態(tài)分子間的能量傳遞、轉(zhuǎn)換等動(dòng)力學(xué)過程在能源、大氣化學(xué)以及生物學(xué)等領(lǐng)域都至關(guān)重要。針對(duì)激發(fā)態(tài)分子反應(yīng)動(dòng)力學(xué)的研究，該研究將聚焦在以下幾方面研究：（1）利用飛秒泵浦-探測技術(shù)等時(shí)間分辨光譜技術(shù)研究光化學(xué)、太陽能轉(zhuǎn)化材料和生物分子檢測中重要體系的激發(fā)態(tài)動(dòng)力學(xué)過程；（2）利用單分子光譜技術(shù)研究單個(gè)超支化分子單光子發(fā)射的特點(diǎn)以及分子內(nèi)各個(gè)分支之間的強(qiáng)或弱相干耦合作用的機(jī)理和規(guī)律；（3）利用實(shí)驗(yàn)方法，研究復(fù)雜體系中如化學(xué)激光體系，大氣化學(xué)體系中重要激發(fā)態(tài)原子分子的傳能以及非絕熱反應(yīng)動(dòng)力學(xué)；（4）利用各種先進(jìn)的實(shí)驗(yàn)方法，研究復(fù)雜體系光解離過程的非絕熱動(dòng)力學(xué)，特別是電子激發(fā)態(tài)與基態(tài)之間，以及激發(fā)態(tài)與激發(fā)態(tài)之間的錐形交叉點(diǎn)非絕熱動(dòng)力學(xué)的研究；（5）發(fā)展新的能夠計(jì)算凝聚態(tài)復(fù)雜分子體系非絕熱過程的動(dòng)力學(xué)理論方法，并利用動(dòng)力學(xué)理論方法來闡述復(fù)雜分子體系的激發(fā)態(tài)動(dòng)力學(xué)機(jī)理。通過該研究，我們將在“分子激發(fā)態(tài)動(dòng)力學(xué)”這個(gè)前沿性科學(xué)問題研究上取得突破性進(jìn)展，取得一批具有重要影響力的創(chuàng)新性研究結(jié)果。

關(guān)鍵詞：分子激發(fā)態(tài) 反應(yīng)動(dòng)力學(xué) 時(shí)間分辨光譜 光解離 復(fù)雜分子體系

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