Spin Dynamics from Atomistic Quantum Simulations

Abstract

Optically active solid-state spin defects are promising candidates for quantum applications, however a unified theoretical framework to predict their spin dynamics at high temperatures is not yet available. Here, using Kubo linear--response theory, we derive expressions of spin-lattice and decoherence times \(T_1\) and \(T_2\) in terms of correlation functions of spin--lattice couplings. We then evaluate \(T_1\) and \(T_2\) from molecular dynamics and spin--lattice interaction time--series generated by state--of--the--art machine learning models trained on {\it ab--initio} data. Finally we measure \(T_1\) times for the NV center in diamond and compare experimental and theoretical results, showing excellent agreement.