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Singlet exciton fission (SF), the conversion of one spin-singlet exciton (S1)into two spin-triplet excitons (T1), could provide a means to overcome theShockley-Queisser limit in photovoltaics. SF as measured by the decay of S1 hasbeen shown to occur efficiently and independently of temperature even when theenergy of S1 is as much as 200 meV less than 2T1. Here, we study films ofTIPS-tetracene using transient optical spectroscopy and show that the initialrise of the triplet pair state (TT) occurs in 300 fs, matched by rapid loss ofS1 stimulated emission, and that this process is mediated by the strongcoupling of electronic and vibrational degrees of freedom. This is followed bya slower 10 ps morphology-dependent phase of S1 decay and TT growth. We observethe TT to be thermally dissociated on 10-100 ns timescales to form freetriplets. This provides a model for "temperature independent", efficient TTformation and thermally activated TT separation.

Ultrafast Triplet Pair Formation and Subsequent Thermally Activated Dissociation Control Efficient Endothermic Singlet Exciton Fission