Low temperature decoherence dynamics in molecular spin systems using the Lindblad master equation

Abstract

Understanding the spin dynamics in low-temperature settings is crucial to designing and optimizing molecular spin systems for use in emerging quantum technologies. At low temperatures, irreversible loss occurs due to ensemble dynamics facilitated by electronic–nuclear spin interactions. We develop a combined open quantum systems and electronic structure theory capable of predicting trends in relaxation rates in molecular spin ensembles. We use the Gorini–Kossakowski–Sudarshan–Lindblad master equation and explicitly include electronic structure information in the decoherence channels. We apply this theory to several molecular systems pertinent to contemporary quantum technologies. Our theory provides a framework to describe irreversible relaxation effects in molecular spin systems with applications in quantum information science, quantum sensing, molecular spintronics, and other spin systems dominated by spin–spin relaxation.