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Several recent electron spin resonance studies have observed a quintetmultiexciton state during the singlet fission process. Here we provide ageneral theoretical explanation for the generation of this state by invoking atime-varying exchange coupling between pairs of triplet excitons, andsubsequently solving the relevant time-varying spin Hamiltonian for a range oftransition times. We simulate experimental ESR spectra and draw qualitativeconclusions about the adiabatic/diabatic transition between triplet pair spinstates.

Fluctuating exchange interactions enable quintet multiexciton formation in singlet fission