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 T1 and T2 in terms of correlation functions of spin--lattice couplings. We then evaluate T1 and T2 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 T1 times for the NV center in diamond and compare experimental and theoretical results, showing excellent agreement.
@article{arxiv.2605.04294,
title = {Spin Dynamics from Atomistic Quantum Simulations},
author = {Enrico Drigo and Marquis M. McMillan and Benjamin Pingault and Yinan Dong and F. Joseph Heremans and David D. Awschalom and Giulia Galli},
journal= {arXiv preprint arXiv:2605.04294},
year = {2026}
}