First-principles Calculation of the Temperature-dependent Transition Energies in Spin Defects

TL;DR

This paper introduces a first-principles computational method to predict how temperature affects the electronic and nuclear spin properties of color centers, crucial for quantum technology applications.

Contribution

The authors develop a novel ab-initio approach to accurately model temperature-dependent properties of spin defects, validated against experimental data for NV centers.

Findings

Good agreement with experimental temperature dependence of NV center properties

Major origin of temperature effects identified as second-order phonon vibrations

Method applicable to various color centers for quantum sensor design

Abstract

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, and in particular temperature, 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 zero phonon line, zero-field splitting, hyperfine interaction, and nuclear quadrupole interaction of color centers. As a testbed, we compare our ab-initio calculation results with experiments in the Nitrogen-Vacancy (NV) center finding good agreement. Interestingly, we identify the major origin of temperature dependence as a second-order effect of phonon vibration. The method is generally applicable to different color centers and provides a theoretical tool for designing high-precision quantum sensors.