Modeling spin relaxation in complex radical systems using MolSpin
Luca Gerhards, Claus Nielsen, Daniel R. Kattnig, P. J. Hore, Ilia A. Solov'yov
Journal of Computational Chemistry
44
1704-1714
2023
abstract
Spin relaxation is an important aspect of the spin dynamics of free radicals and can have asignificant impact on the outcome of their spin-selective reactions. Examples range from the use of radicals as spin qubits in quantum information processing to the radical pair reactions in proteins that may allow migratory birds to sense the direction of the Earth's magnetic field. Accurate modeling of spin relaxation however, is non-trivial. Bloch–Redfield–Wangsness theory derives a quantum mechanical master equation from system-bath interactions in the Markovian limit that provides a comprehensive framework for describing spin relaxation. Unfortunately, the construction of the master equation is system-specific and often resource-heavy. To address this challenge, we introduce a generalized and efficient implementation of BRW theory as a new feature of the spin dynamics toolkit MolSpin which offers an easy-to-use approach for studying systems of reacting radicals of varying complexity.