First-Principles Calculation of the Temperature-Dependent Transition Energies in Spin Defects

Spin qubits associated with color centers are promising platforms for various quantum technologies. However, to be deployed in robust quantum devices, the variations of their intrinsic properties with the external conditions, in particular temperature and strain, should be known with high precision. Unfortunately, a predictive theory on the temperature dependence of the resonance frequency of electron and nuclear spin defects in solids remains lacking. In this work, we develop a first-principles method for the temperature dependence of the zero-field splitting, hyperfine interaction, and nuclear quadrupole interaction of color centers. As a testbed, we compare our ab initio calculations with experiments for the nitrogen-vacancy (NV^-) center in diamond, finding good agreements. We identify the major origin of the temperature dependence as a second-order effect of dynamic phonon vibrations, instead of the thermal-expansion strain. The method can be applied to different color centers and provides a theoretical tool for designing high-precision quantum sensors.