Site-Specific Time-Resolved Multidimensional Spectroscopy of Electron Transfer Dynamics

在这个由化学部门化学结构和动力学项目A资助的项目中，密歇根大学的Kevin Kubarych教授和他的研究生正在开发de novo（“从零开始”）蛋白质来研究电子的基本运动。电子转移过程对生命至关重要，在开发新方法以获取能量并将其转化为有用形式的过程中，它们构成了许多最紧迫挑战的基础。该项目通过一系列研讨会和会议促进光谱工具产生的研究机会，例如在研究中使用的工具。Kubarych教授的研究小组使用先进的超快激光光谱方法，利用设计的从头金属酶支架实时可视化电子转移。合成和光谱相结合的方法提供了灵活性，以改变电子供体和受体的位置，并增加加速桥接侧链。补充这种大分子设计策略的是Kubarych实验室开发的基于多维光谱的光谱工具集。该项目还使用了nsf资助的合作设施，超快多维光谱学实验室（LUMOS）。LUMOS正在被开发用于跟踪电子转移和其他光触发反应，从飞秒到秒的波长范围从紫外、可见光到红外。这种极宽的时间和频率范围对于监测电荷通过工程蛋白时结构和动力学的变化至关重要。

In this project funded by the Chemical Structure and Dynamics Program A of the Chemistry Division, Professor Kevin Kubarych of the University of Michigan and his graduate students are developing de novo ("from scratch") proteins to study the fundamental motion of electrons. Electron transfer processes are essential to life, and they underlie many of the most pressing challenges in developing new methods to harvest energy and convert it into useful forms. The project promotes research opportunities arising from spectroscopic tools such as used in the research via a series of workshops and meetings.Professor Kubarych's research group uses advanced ultrafast laser spectroscopy methods to visualize electron transfer in real time using designed de novo metalloenzyme scaffolds. The combined synthetic and spectroscopic approach offers the flexibility to change the location of the electron donor and acceptor, and to add accelerating bridging side chains. Complementing this macromolecular design strategy is a spectroscopic toolset based on multidimensional spectroscopy that has been developed in the Kubarych lab. The project also uses a collaborative NSF-funded facility, the Laboratory for Ultrafast Multidimensional Optical Spectroscopy (LUMOS). LUMOS is being developed to track electron transfer and other phototriggered reactions from femtoseconds to seconds at wavelengths ranging from the UV and visible to the infrared. This extremely broad temporal and frequency range is essential to monitor changes in structure and dynamics as the charge moves through the engineered protein.