Spins in molecular films can be observed in the ground state in the form of free radials or paramagnetic ions. They can also be obtained in the photoexcited state, and harnessed to improve photoemission yields in OLEDs or efficiency in photovoltaics. One particularly intriguing phenomenon is singlet fission in pentacene, where a single photon absorbed for a singlet excitation can be converted into two triplets, potentially boosting efficiency in solar cells. This presentation will focus on elucidating the correlation between molecular structure and couplings of spins obtained by singlet photoexcitation. The impact of intermolecular interactions will be probed via pentacene dilution within an insulating matrix, and temperature-dependent spectroscopies including transient electron paramagnetic resonance. The impact of spin coupling on future applications will be considered.
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