TRANSIENT IR STUDIES OF PROTON COUPLED ELECTRON TRANSFER

这个子项目是许多研究子项目中的一个 由NIH/NCRR资助的中心赠款提供的资源。子项目和 研究者（PI）可能从另一个NIH来源获得了主要资金， 因此可以在其他CRISP条目中表示。所列机构为 研究中心，而研究中心不一定是研究者所在的机构。 我们打算追求的动力学相关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瞬态光谱。光学泵浦-探测、光学泵浦/红外探测和动力学斯托克斯位移实验将与瞬态光学泵浦-探测实验等实验相关联。 这项工作将描绘结构-功能关系，设计结合供体-间隔区-受体（D-Sp-A）超分子和共价连接的多辅因子组件。 虽然这些系统具有降低的结构复杂性，但它们能够独立地调节围绕D和A的局部静电力。 我们将研究光诱导PCET反应在这样的系统中使用光泵/光探针和可见光泵/红外探针光谱方法，并与所观察到的动态与特定的响应与特定的结构。

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.