Ultrafast Dynamics Occurring in the Ground States of Transition Metal Ccmplexes

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In this project, funded by the Chemical Structure, Dynamics, and Mechanisms B Program of the Chemistry Division, Professor Clifford Kubiak of the Department of Chemistry and Biochemistry at the University of California San Diego is developing new assemblies of metal complexes that undergo fast electron transfer (ET) reactions. Electron transfer (ET) is the basis of operation of every electronic device. ET research can elucidate methods for efficient conversion of light to electrons and, subsequently, usable and storable chemical energy. This NSF-funded project investigates a new generation of mixed-valent complexes to study the behavior of electronic delocalization in molecular systems. The ramifications of these findings can extend to the development of integrated circuits, quantum computing, and artificial photosynthesis. In tandem with this project, Professor Kubiak’s group is also dedicated to community outreach and science education, engaging and involving K-12 and undergraduate students in cutting edge fundamental science.Mixed-valent trinuclear oxo-bridged clusters have proven to be valuable model systems for the development and understanding of the factors that control the rates, switching location, and polarization of ground state electron transfer on the ultrafast (picosecond) timescale using infrared spectroscopy and electrochemistry to probe these phenomena. The most recent support period informed several key aims for future research, including: (i) covalent attachment of mixed-valent complexes to electrode surfaces and measurement of the influence of electric fields on mixed-valent complexes potential energy surfaces; (ii) extending the study of electric field driven ET towards driving chemical reactions important to catalysis; (iii) the study of mixed-valent complexes joined by chiral bridges to understand interactions between chiral molecules and spin; and (iv) the preparation and study of high-spin mixed-valent iron clusters.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.