The development of spin qubits for quantum technologies requires their protection from the main source of finite-temperature decoherence: atomic vibrations. Here we eliminate one of the main barriers to the progress in this field by providing a complete first-principles picture of spin relaxation that includes up to two-phonon processes. Our method is based on machine learning and electronic structure theory and makes the prediction of spin lifetime in realistic systems feasible. We study a prototypical vanadium-based molecular qubit and reveal that the spin lifetime at high temperature is limited by Raman processes due to a small number of THz intramolecular vibrations. These findings effectively change the conventional understanding of spin relaxation in this class of materials and open new avenues for the rational design of long-living spin systems.
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