Ultrafast one- and two-dimensional infrared spectroscopic studies of electronic state dynamics in organometallics

在化学系化学结构、动力学和机理计划的支持下，加州大学伯克利分校的查尔斯·B·哈里斯教授和他的研究小组将使用超快一维和二维红外光谱来研究金属有机体系中电子态的动力学。这项工作建立在该小组广泛经验的基础上，并将探索电子跃迁和转移的方式，无论是光化学诱导的还是处于热平衡的，都决定了有机金属配合物对催化相关体系的反应性。这些实验将在分子尺度装置的背景下加深对分子内电子转移的理解，阐明自旋态变化和外部重原子效应对反应动力学的作用，并阐明新型二氧化碳还原催化剂的动力学。超快红外光谱为深入了解这些重要的反应类别提供了完美的工具。此外，这项研究将受益于一种多方面的方法，不仅涉及实验分子光谱，还包括合成和理论。这一环境得到了与其他机构教职员工的合作的补充。学生(包括研究生和本科生)将从这种多学科研究环境中受益。最后，哈里斯小组参与了各种社区外展和教育活动，以促进更广泛的公众对化学和科学的理解和欣赏。

With the support of the Chemical Structure, Dynamics and Mechanisms Program in the Division of Chemistry, Professor Charles B. Harris of the University of California, Berkeley and his research group will use ultrafast one- and two-dimensional infrared spectroscopies to study the dynamics of electronic states in organometallic systems. This work builds upon the group's extensive experience and will explore the ways in which electronic transitions and transfers, both photochemically-induced and at thermal equilibrium, dictate the reactivity of organometallic complexes for catalytically-relevant systems. These experiments will improve the current understanding of intramolecular electron transfer in the context of molecular-scale devices, clarify the role of spin state changes and external heavy atom effects on reaction dynamics, and elucidate the dynamics of novel CO2 reduction catalysts. Ultrafast infrared spectroscopy provides the perfect tool for developing a deep understanding of these important classes of reactions.Additionally, this research will benefit from a multi-faceted approach involving not only experimental molecular spectroscopy, but also synthesis and theory. This environment is supplemented by collaborations with faculty at other institutions. Students (both graduate and undergraduate) will benefit from this multi-disciplinary research setting. Finally, the Harris group is engaged in a variety of community outreach and education activities that promote a broader public understanding and appreciation for chemistry and science in general.