Multielectron Photoinduced Charge Transfer Chemistry in a Molecular System

普林斯顿大学化学系的Andrew B. Bocarsly博士受到无机、生物无机和有机金属化学项目的支持，从事多电子电荷转移反应的光化学和光物理研究。多金属氰基桥接Pt（IV）体系在光激发后发生了双电子电荷转移反应。为了更好地理解主控制过程，将对该系统进行详细的研究。初级光产物的电子和分子结构将用高速激光光谱测定。与电荷转移态相关的离域程度将被确定，以及溶剂的作用。这些信息将用于合成新的氰基桥接多核体系，以便对观察到的电荷转移化学提供分子控制。电子被光激活后被调动的材料在技术上是重要的。在这个项目中，将确定与光反应对一系列化合物的影响的结构细节。将尝试延长材料的寿命，以便进行进一步的光活化。这一基础研究项目将提高利用太阳能形成有用燃料和精细化学品以及开发非线性光学材料的能力。

Dr. Andrew B. Bocarsly of the Chemistry Department, Princeton University, is supported by the Inorganic, Bioinorganic, and Organometallic Chemistry Program for research on the photochemistry and photophysics of multielectron charge transfer reactions. A multimetal cyano-bridged Pt(IV) system has been shown to undergo a two-electron charge transfer reaction after photoexcitation. This system will be studied in detail in order to gain better understanding of the primary controlling process. The electronic and molecular structure of the primary photoproduct will be determined using high speed laser spectroscopy. The degree of delocalization associated with the charge transfer state will be determined, as well as the role of solvent. This information will be used to synthesize new cyano-bridged multinuclear systems in order to provide molecular control over the observed charge transfer chemistry. Materials in which electrons are mobilized after being activated by light are technologically important. In this project, the structural details of the effect of reaction with light on a series of compounds will be determined. Attempts will be made to extend the lifetime of the material so that further photoactivation can take place. This fundamental research project will improve capability to utilize solar energy for the formation of useful fuels and fine chemicals and to develop nonlinear optical materials.