CAREER: SusChEM: Computational Studies of Light-Induced Dynamics in First-Row Transition Metal Complexes

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In this CAREER project funded by the Chemical Structure, Dynamics & Mechanism B Program of the Chemistry Division, Professor Elena Jakubikova of the Department of Chemistry at North Carolina State University investigates how transition metal complexes based on earth-abundant metals interact with light. The goal of this project is to utilize computer modeling to obtain a deeper understanding of structure-property relationships in such complexes, so that new chromophores, photocatalysts or photomagnetic materials may be designed. The project lies at the interface of computational, inorganic, and physical chemistry, and is therefore well positioned to introduce computational chemistry as a valuable tool to a wide range of students at the high school, undergraduate and graduate levels. Collection of dyes in the Max A. Weaver Dye Library at North Carolina State University is used to motivate the research and educational activities of high school and undergraduate students. The students contribute developing a set of data for the library to benchmark computational methodologies for calculations of visible absorption spectra and to screen dyes for use as chromophores in dye-sensitized solar cells.The rational design of chromophores and photocatalysts based on first row transition metal complexes relies on the fundamental knowledge of how these complexes absorb and dissipate light. In particular, understanding the mechanisms of nonradiative decay processes, such as internal conversion and intersystem crossing, is key to our ability to control excited state properties of these systems. The goal of this project is to obtain a better theoretical understanding of the mechanism of nonradiative decay in first row transition metal complexes, so that a more rational approach to the development of efficient chromophores, photocatalysts, and photomagnetic materials based on earth-abundant metals can be taken. Specifically, the project focuses on structural factors that facilitate the ultrafast intersystem crossing events in iron-based complexes. The project involves computational studies on a series of octahedral as well as low coordinate iron complexes utilizing density functional theory, time-dependent density functional theory, nonadiabatic transition state theory, and nonadiabatic surface hopping dynamics. Minority and economically disadvantaged students are recruited through the existingrelationships with the NC Project SEED program and the NSF-Research Experiences for Undergraduates Program in the Department of Chemistry. Local high school teachers are provided with the tools and expertiseto develop and implement their own computational chemistry modules into the Advanced Placement Chemistry curriculum using the North Carolina High School Computational Chemistry Server.