Intersystem Crossing and Triplet Fusion in Singlet-Fission-Dominated Rubrene-Based OLEDs Under High Bias Current

Singlet fission is usually the only reaction channel for excited states in rubrene-based organic light-emitting diodes (OLEDs) at ambient temperature. Intriguingly, we discover that triplet fusion (TF) and intersystem crossing (ISC) within rubrene-based devices begin at moderate and high current densities (j), respectively. Both processes enhance with decreasing temperature. This behavior is discovered by analyzing the magneto-electroluminescence curves of the devices. The j-dependent magneto-conductance, measured at ambient temperature indicates that spin mixing within polaron pairs that are generated by triplet-charge annihilation (TQA) causes the occurrence of ISC, while the high concentrations of triplets are responsible for generating TF. Additionally, the reduction in exciton formation and the elevated TQA with decreasing temperature may contribute to the enhanced ISC at low temperatures. This work provides considerable insight into the different mechanisms that occur when a high density of excited states exist in rubrene and reasonable reasons for the absence of EL efficiency roll-off in rubrene-based OLEDs.