The Impact of Ligand Field Symmetry on Molecular Qubit Coherence

Abstract

Developing quantum bits (qubits) exhibiting room temperature electron spin coherence is a key goal of molecular quantum information science. Here we develop a simple and powerful model for predicting relative T<sub>1</sub> coherence times in transition metal complexes from dynamic ligand field principles. By considering the excited state origins of ground state spin-phonon coupling, we derive group theory selection rules governing which vibrational symmetries can induce decoherence. Thermal weighting of the coupling terms produces surprisingly good predictions of experimental T<sub>1</sub> trends as a function of temperature and explains previously confounding features in spin-lattice relaxation data. We use this model to evaluate experimental relaxation rates across S = ½ transition metal qubit candidates with diverse structures, gaining new insights into the interplay between spin-phonon coupling and molecular symmetry. This methodology elucidates the specific vibrational modes giving rise to decoherence, suggesting symmetry-based design strategies and providing insight into the origin of room temperature coherence in transition metal complexes.