Fluctuating exchange interactions enable quintet multiexciton formation in singlet fission

Abstract: Several recent electron spin resonance studies have observed a quintet multiexciton state during the singlet fission process. Here we provide a general theoretical explanation for the generation of this state by invoking a time-varying exchange coupling between pairs of triplet excitons, and subsequently solving the relevant time-varying spin Hamiltonian for a range of transition times. We simulate experimental ESR spectra and draw qualitative conclusions about the adiabatic/diabatic transition between triplet pair spin states.