High spin transition metal complexes hold significant potential for scaling molecule-based processors for quantum computation. The practical implementation of such species is elusive, however, because high-spin qubits exhibit fragile superpositions and are not suitable for long computational cycles. Therefore, design principles for the syntheses of stable high-spin qubits are extremely useful from the standpoint of practical use. Toward this end, we are using synthetic inorganic chemistry to probe the influence of specific structural and electronic features of transition metal complexes on superposition stability. Our synthetic strategy is guided primarily by the desire to minimize the impact of nuclear spin, which are potent instigators of superposition collapse. Thus, all employed ligand sets are composed only of elements that have high natural abundances of nuclear spin-free isotopes. We will present pulsed electron paramagnetic resonance investigations of the impact of the ligand set on the stability of the electronic spin superpositions in a series of high-spin transition metal complexes. Our results demonstrate the importance of thermal processes on decoherence in high-spin species even in rigorously nuclear spin-free molecules.

Thermally mediated decoherence in high-spin, nuclear spin-free transition metal complexes

251st National Meeting (2016)

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