TRANSIENT IR STUDIES OF PROTON COUPLED ELECTRON TRANSFER

这个子项目是许多研究子项目中利用 资源由NIH/NCRR资助的中心拨款提供。子项目和 调查员(PI)可能从NIH的另一个来源获得了主要资金， 并因此可以在其他清晰的条目中表示。列出的机构是 该中心不一定是调查人员的机构。 我们打算进行的与动力学相关的实验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瞬变光谱。光抽运探测实验、光抽运/红外探测实验和动力学斯托克斯漂移实验将与瞬变光学抽运探测实验相关联。 这项工作将描绘结构-功能关系工程，以结合施主-间隔物-受体(D-Sp-A)超分子和共价连接的多辅助因子组件。虽然这些体系的结构复杂性降低了，但它们能够独立地调制D和A周围的局部静电力。我们将使用光泵/光探测器和可见光泵浦/红外探测光谱方法来研究这类系统中的光诱导PCET反应，并将观察到的动力学与特定结构的特定响应联系起来。

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 types of dynamics-correlated experiments that we intend to pursue will utilize state-of-the-art experimental methodologies and instrumentation to study molecular transient spectroscopy 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 experiments. This work will delineate structure-function relationships engineered to bind donor - spacer - acceptor (D-Sp-A) supermolecules and covalently linked multi-cofactor assemblies. While these systems possess reduced structural complexity, they enable independent modulation of the local electrostatic forces that surround D and A. We will examine photoinduced PCET reactions in such systems using optical pump / optical probe and visible pump / IR probe spectroscopic methods, and correlate the observed dynamics with specific responses with specific structures.