基于压力的分子荧光共振能量转移动力学研究

Molecular fluorescence resonance energy transfer is currently one of the frontier areas of atomic and molecular physics. This project combines femtosecond time-resolved transient absorption spectroscopy with the technology of diamond anvil high-pressure cells and studies ultrafast dynamics of molecular fluorescence resonance energy transfer in liquid phase systems. Fluorescence resonance energy transfer efficiency has a strong dependence on the distance between donor and acceptor, so the pressure is used to directly change the distance between donor and acceptor, and the femtosecond time-resolved spectroscopy technique is used to observe fluorescence resonance energy transfer process in real time. In theory, combined with the first-principle quantum computing method, the ground state and excited state structure, charge distribution and so on of molecules based on pressure effect are analyzed and discussed in depth so as to obtain the effect of pressure on the details of ultrafast fluorescence resonance energy transfer process. This project aims to reveal the physical mechanism of the effect of pressure on the ultrafast process of intramolecular and intermolecular fluorescence resonance energy transfer and to explore the application of this physical effect in the control of ultrafast dynamics for fluorescence resonance energy transfer process.

分子荧光共振能量转移是当前原子与分子物理学的前沿研究领域之一。本项目将飞秒时间分辨瞬态吸收光谱技术与金刚石对顶砧高压技术相结合，针对液相体系中分子荧光共振能量转移超快动力学过程进行研究。荧光共振能量转移效率对给体与受体间距离具有很强的依赖性，利用压力直接改变给体与受体间的距离，并采用飞秒时间分辨光谱技术对分子荧光共振能量转移过程进行实时观测。在理论上，结合第一性原理的量子计算方法，对基于压力效应的分子基态和激发态结构、电荷分布等进行深入分析与探讨，从而获得压力对荧光共振能量转移超快动力学过程影响的详细信息。本项目旨在揭示压力对于分子内和分子间荧光共振能量转移超快过程影响的物理机理，并进一步探索压力这一物理效应在荧光共振能量转移超快动力学过程控制中的应用途径。

本项目研究了高压对分子激发态共振能量转移过程的调控，对理解和认识极端条件下分子激发态过程具有重要的意义。项目执行期间，我们完善了高压飞秒瞬态吸收光谱技术平台，并开展了对高压下共振能量转移动力学过程的实时观测；理论上结合第一性原理的量子计算方法，对分子基态和激发态结构、光谱以及电荷分布等进行深入分析与探讨，从而获得压力对荧光共振能量转移超快动力学过程影响的详细信息，揭示压力对于激发态分子间共振能量转移超快过程影响的物理机理。项目执行期间，项目负责人作为通讯作者在包括J.Phys.Chem.Lett.,Opt.Express,J.Mater.Chem.C.等原子与分子物理和化学物理领域知名学术期刊上发表SCI收录论文27篇。项目负责人多次参加国内外学术会议并作邀请或口头报告。项目执行期间，培养原子与分子物理专业获博士学位研究生7名，获硕士学位研究生5名。项目研究提升了我们对极端条件下分子激发态动力学特性的理解，也为进一步的研究工作打下坚实的基础。

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