COHERENT PHENOMENA IN ULTRAFAST BIOLOGICAL PROCESSES

该子项目是利用NIH/NCRR资助的中心赠款提供的资源的许多研究子项目之一。子项目和研究者（PI）可能从另一个NIH来源获得主要资金，因此可以在其他CRISP条目中表示。所列机构为中心，不一定是研究者所在机构。该研究项目的主要目标是利用超快振动光谱提供的独特信息，以发展与生物学相关的超快过程的基本见解。因此，我们打算（1）确定电子转移中涉及的中间态的关键振动特征，（2）确定强耦合供体-受体系统中电荷迁移的程度，（3）检查反应的动力学，如超快质子耦合电子转移，其中快速键断裂和键形成事件发生在类似于电荷迁移的时间尺度上，（4）理解激发态发色团核动力学的性质，（5）探索离域多色素系统中电子激发态的性质。 我们打算追求的动力学相关ET实验的类型将利用最先进的实验方法和仪器来研究快速，亚纳秒时间尺度上的分子振动。光泵浦探测、光泵浦/红外探测和动力学斯托克斯位移实验将与瞬态光泵浦探测实验、瞬态光泵浦探测实验等实验相关联。

This subproject is one of many research subprojects utilizing the resources provided by a Center grant funded by NIH/NCRR. The subproject and investigator (PI) may have received primary funding from another NIH source, and thus could be represented in other CRISP entries. The institution listed is for the Center, which is not necessarily the institution for the investigator. The primary goal of this research project is to exploit the unique information that ultrafast vibrational spectroscopy provides to develop fundamental insights into ultrafast processes relevant to biology. We thereby intend to (1) identify key vibrational signatures of intermediate states involved in electron transfer, (2) ascertain the extent to which charge migrates in strongly coupled donor-acceptor systems, (3) examine the dynamics of reactions such as ultrafast proton-coupled electron transfer in which fast bond-breaking and bond-forming events occur on time scales similar to charge migration, (4) understand the nature of excited-state chromophore nuclear dynamics, and (5) probe the nature of electronically excited states in delocalized, multipigment systems. The types of dynmaics-correlated ET experiments that we intend to pursue will utilize state-of-the-art experimental methodologies and instrumentation to study molecular vibrations on fast, sub-nanosecond time scales. Optical pump-probe, optical-pump/infrared-probe and dynamics Stokes shift experiments will be correlated with experiments such as transient optical pump-probe experime