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Molecular electronic spins represent one of the most promising buildingblocks for the design of quantum computing architectures. However, theadvancement of this technology requires the increase of spin lifetime atambient temperature. Spin-phonon coupling has been recognized as the keyinteraction dictating spin relaxation at high temperature in molecular crystalsand the search for chemical-design principles to control such interaction are afundamental challenge in the field. Here we present a multi-referencefirst-principles analysis of the g-tensor and the spin-phonon coupling in aseries of four exa-coordinate Vanadium(IV) molecular complexes, where thecatecholate ligand donor atom is progressively changed from Oxygen to Sulphur,Selenium and Tellurium. A ligand field interpretation of the multi-referenceelectronic structure theory results made it possible to rationalize thecorrelation between the molecular g-shifts and the average spin-phonon couplingcoefficients, revealing the role of spin-orbit coupling, chemical bondcovalency and energy splitting of d-like orbitals in spin relaxation. Our studyreveals the simultaneous increase of metal-ligand covalency and electronicexcited state energy separation as key elements of an optimal strategy towardslong spin-lattice lifetimes in molecular qubits.

Ligand-field contributions to spin-phonon coupling in a family of Vanadium molecular qubits from multi-reference electronic structure theory