Effects of Molecular Topology and Environment on Dynamics of Electron Transfer Processes in Porphyrin-Fullerene Hybrid Materials

通过这个奖项，有机和大分子项目支持纽约大学化学系大卫·i·舒斯特教授的工作。该研究将继续PI对含有卟啉和富勒烯基团的供体-受体系统溶液中光诱导电子转移反应动力学的研究，作为这些基团的拓扑和空间关系的函数。目的是了解色团间距离、分子构象、拓扑关系和环境如何影响能量转移、电荷分离和电荷重组过程的速率。要研究的材料包括共价连接的体系，主要是那些具有可以作为分子线的炔连接剂的体系，以及机械连接的体系，即轮烷和链烷。多组分系统，其中光诱导的能量和电子转移过程逐步发生，就像在自然界一样，将发展为光合模型。合成技术的最新进展将使构造结构比以前用于此类研究的材料更复杂、更有趣。这些材料暴露在太阳光谱区的激发下所发生的过程的详细机制，将由PI在纽约大学的实验室以及时间分辨光谱和磁共振技术专家的合作者的实验室进行研究。这项工作将由学生和博士后进行，他们将获得在新型纳米材料的合成、分离和表征方面的经验。计算研究，在PI的实验室以及与纽约大学的理论同事，也将发挥作用。这项研究的一个重要方面是本科生的广泛参与，从大二或大三开始，在特殊情况下甚至是大一。这些学生将接受有机化学前沿研究方面的培训，从基本原理和化学文献衍生的项目概念，到使用现代合成、分析和光谱方法执行。所有同事都将接受光化学、光物理和材料科学的基础教育。这次培训将为研究生学习和职业发展做很好的准备。从实际的角度来看，用于储能的太阳能电池将由本研究过程中发现的有前途的材料合作开发。

With this award, the Organic and Macromolecular Program supports the work of Professor David I. Schuster, of the Department of Chemistry at New York University. This research will continue the PI's investigations of the dynamics of photoinduced electron transfer reactions in solution in donor-acceptor systems incorporating porphyrin and fullerene moieties, as a function of the topological and spatial relationships of these groups. The goal is to gain understanding of how interchromophoric distance, molecular conformation, topological relationships and environment affect the rates of energy transfer, charge separation and charge recombination processes. The materials to be studied included covalently-linked systems, predominantly those with alkyne linkers which can act as molecular wires, as well as mechanically-linked systems, i.e., rotaxanes and catenanes. Multicomponent systems, in which photoinduced energy and electron transfer processes take place stepwise, as in nature, will be developed as photosynthetic models. Recent advances in synthetic techniques will allow construction of structurally more complex and interesting materials than those previously available for such studies. The detailed mechanisms of the processes occurring upon exposure of these materials to excitation in the solar spectral region will be elaborated by studies in the PI's lab at NYU and in the laboratories of collaborators who are experts in time-resolved spectroscopic and magnetic resonance techniques.The work will be carried out by students and postdoctoral fellows, who will gain experience in the synthesis, isolation and characterization of novel nanoscale materials. Computational studies, in the PI's lab as well as with theory colleagues on the NYU faculty, will also play a role. An important aspect of this research will be the extensive involvement of undergraduates, beginning in their sophomore or junior years, and in special cases even as freshmen. These students will receive training in cutting-edge research in organic chemistry, from project conception derived from basic principles and the chemical literature, to execution using contemporary synthetic, analytic and spectroscopic methods. All coworkers will receive grounding in photochemical, photophysical and material sciences. This training will be excellent preparation for graduate studies and career development. From a practical point of view, solar cells for energy storage will be developed collaboratively from promising materials discovered in the course of this research.