Comparative Study of the High Harmonic Spectra of Transition Metal Compounds

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Advancements in laser technology have opened new frontiers in the study of high harmonic generation (HHG), a phenomenon where intense laser light interacting with materials produces higher frequencies of light. This project aims to harness HHG to better understand the chemistry of transition metal compounds, which are essential in various chemical processes and have extensive industrial applications. Transition metal compounds have intriguing properties, partly due to their complex electronic structures. By exploring the HHG spectra of transition metal compounds, this research contributes to advancing our understanding of these materials, which can have wide-ranging implications for innovations in chemistry and materials science. Additionally, this project includes educational components that will serve the national interest by training the next generation of scientists. It integrates cutting-edge research into classrooms and actively engages undergraduate students, providing them with invaluable experience. Through collaborations with local schools, this project also seeks to inspire younger students and foster a community-wide appreciation for science.This project focuses on examining the HHG spectra of transition metal compounds containing carbonyl, cyanide, and chloride groups. The study employs time-dependent density functional theory (TDDFT) calculations to investigate several compounds such as Ni(CO)4, V(CO)6, Ni(CN)2, Ni(CN)4^3-, and NiCl4^2-. The analyses will encompass understanding the variations in the HHG spectra in terms of the metal's properties, ligands, spin states, and coordination geometries. Furthermore, the project will probe the deviations from the high harmonic cutoff law, analyze resonance-enhanced high harmonic emissions below the ionization potential, and explore charge transfer between the metal and ligands. This comprehensive approach will help in understanding how the phase relations of multiple electrons on different trajectories can deviate from the single-active-electron (SAE) predictions in transition metal compounds. Moreover, it involves systematic benchmarking and improvement of the TDDFT methods developed by the PI and collaborators, which can further deepen insights into complex electronic structures and multi-electron dynamics in transition metal compounds.This project is jointly funded by the Atomic, Molecular, and Optical Physics Theory Program and the Established Program to Stimulate Competitive Research (EPSCoR).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.