Monte-Carlo wavefunction approach for the spin dynamics of recombining radicals

Abstract

We adapt the Monte-Carlo wavefunction (MCWF) approach to treat the open-system spin dynamics of radical pairs subject to spin-selective recombination reactions. For these systems, non-Lindbladian master equations are widely employed, which account for recombination via the non trace-preserving Haberkorn superoperator in combination with reaction-dependent exchange and singlet–triplet dephasing terms. We show that this type of master equation can be accommodated in the MCWF approach, by introducing a second type of quantum jump that accounts for the reaction simply by suitably terminating the propagation. In this way, we are able to evaluate approximate solutions to the time-dependent radical pair survival probability for systems that have been considered untreatable with the master equation approach until now. We explicate the suggested approach with calculations for radical pair reactions that have been suggested to be relevant for the quantum compass of birds and related phenomena.