Singlet-triplet fission is a multiexciton generation process in which two triplets or charge carriers are generated for each absorbed photon − a process which may substantially enhance the efficiency of solar cells. Using temperature-dependent broadband optical pump-probe spectroscopy we provide experimental evidence that the fission process in pentacene is governed by the internal dynamics of a double dark state with biexciton char- acter. The biexciton formation occurs on sub-ps timescales and is accompanied by delayed blueshifted superradiance at low temperatures due to defects and quantum confinement.
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