Electron Dynamics in Molecular Qubits and Catalytic Films

Author: Mirzoyan, Ruben

Year: 2025

Degree: Dissertation (Ph.D.)

Advisor: Hadt, Ryan G.

Committee Members: Gray, Harry B.; Hadt, Ryan G.; See, Kimberly; Winkler, Jay Richmond

Option: Chemistry

DOI: 10.7907/mcq5-js86

Abstract

Two significant areas within molecular and materials chemistry are explored: spin-phonon coupling in molecular qubits and electrocatalysis in cobalt oxyhydroxide thin films, detailed over four chapters and an appendix. The first chapter reviews advancements in molecular quantum information science, focusing on decoherence mechanisms in transition metal complex-based qubits, and introduces a dynamic ligand field model that categorizes decoherence regimes and designs qubits for various environments. The second chapter develops and enhances a ligand field theory model to quantify spin-phonon interactions in transition metal complexes, correlating theoretical insights with experimental data to improve quantum coherence in molecular qubits. The third chapter investigates the electron transport and dynamic defect states in cobalt-phosphate and cobalt-borate oxyhydroxide films, crucial for understanding their photoexcited states in oxygen evolution catalysis. The fourth chapter presents a novel magneto-electrochemical setup that quantifies magnetoenhancement in electrocatalytic current for water splitting, highlighting the potential of magnetic fields in enhancing electrocatalytic processes. This work provides both a physical inorganic framework and experimental insights for ongoing and future developments in molecular quantum information science and energy conversion.

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