Functional materials that change spin, optical, and charge state upon application of external stimuli (light, electric Keld, or magnetic Keld) are central to the development of non-volatile memory technologies, spintronics devices, and sensors for quantum information science (QIS). Within the context of quantum information science, quantum computing, communications, and sensors all rely on the fundamental unit of a qubit. In general, a qubit possesses at least two well-deKned quantum states that can be prepared and addressed independently. Qubits can interact to generate an inKnite number of states leading to exciting new possibilities for data processing, storage, and sensing at the quantum level. The concept of coupling optically-bistable photochromic ligands to electronically-bistable metal complexes is an enticing strategy for controlling the electronic structure and lifetime of optically-gated functional materials. The electronic coupling between metal center and photochrome states, however, is complex, and fundamental studies towards elucidating the primary mechanism of electronic coupling are central to the expansion of this strategy towards other spin-based systems. The immediate goal of this work is the creation of a generalized strategy for molecular qubits that can be controlled with light under ambient conditions to enable embedded resistive memory devices and sensors with signiKcantly decreased energy demand.