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

Paramagnetic defects in diamond and hexagonal boron nitride possess a combination of spin and optical properties that make them prototypical solid-state qubits. Despite the coherence of these spin qubits being critically limited by spin-phonon relaxation, a full understanding of this process is not yet available. Here we apply ab initio spin dynamics simulations to this problem and quantitatively reproduce the experimental temperature dependence of spin relaxation time and spin coherence time. We demonstrate that low-frequency two-phonon modulations of the zero-field splitting are responsible for spin relaxation and decoherence, and point to the nature of vibrations in 2-dimensional materials as the culprit for their shorter coherence time. These results provide an interpretation to spin-phonon decoherence in solid-state paramagnetic defects, offer a strategy to correctly interpret experimental results, and pave the way for the accelerated design of spin qubits.

Automated summary

Paramagnetic defects in diamond and hexagonal boron nitride exhibit spin and optical properties that make them ideal for solid-state qubits. However, their coherence is limited by spin-phonon relaxation, and a complete understanding of this process is lacking. In this study, we use ab initio spin dynamics simulations to successfully reproduce the experimental temperature dependence of spin relaxation and coherence time. We find that low-frequency two-phonon modulations are responsible for spin relaxation and decoherence, and attribute the shorter coherence time to the vibrations in 2-dimensional materials. These findings provide insights into spin-phonon decoherence in solid-state qubits and facilitate the design of more efficient spin qubits.