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.

arXiv comment7 pages, 8 figures, typos corrected

References in corpus (3)

• QuTiP 2: A Python framework for the dynamics of open quantum systems
• Multiple Quintets via Singlet Fission in Ordered Films at Room Temperature
• Diagrammatic Exciton Basis Theory of the Photophysics of Pentacene Dimers

Cited by in corpus (6)

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• Singlet Fission Photovoltaics: Progress and Promising Pathways
• Triplet-Pair Spin Signatures from Macroscopically Aligned Heteroacenes in an Oriented Single Crystal
• Heterogeneous Singlet Fission in a Covalently Linked Pentacene Dimer
• Spin-dependent recombination mechanisms for quintet bi-excitons generated through singlet fission
• Optimisation of ultrafast singlet fission in 1D rings towards unit efficiency