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Paramagnetic defects in diamond and hexagonal boron nitride possess a uniquecombination of spin and optical properties that make them prototypicalsolid-state qubits. Despite the coherence of these spin qubits being criticallylimited by spin-phonon relaxation, a full understanding of this process is notyet available. Here we apply ab initio spin dynamics simulations to thisproblem and quantitatively reproduce the experimental temperature dependence ofspin relaxation time and spin coherence time. We demonstrate that low-frequencytwo-phonon modulations of the zero-field splitting are responsible for spinrelaxation and decoherence, and point to the nature of vibrations in2-dimensional materials as the culprit for their shorter coherence time. Theseresults provide a novel interpretation to spin-phonon decoherence insolid-state paramagnetic defects, offer a new strategy to correctly interpretexperimental results, and pave the way for the accelerated design of new spinqubits.

Spin-phonon decoherence in solid-state paramagnetic defects from first principles