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.

Guest concentration, bias current, and temperature-dependent sign inversion of magneto-electroluminescence in thermally activated delayed fluorescence devices.

Non-emissive triplet excited states in devices that undergo thermally activated delayed fluorescence (TADF) can be up-converted to singlet excited states via reverse intersystem crossing (RISC), which leads to an enhanced electroluminescence efficiency. Exciton-based fluorescence devices always exhibit a positive magneto-electroluminescence (MEL) because intersystem crossing (ISC) can be suppressed effectively by an external magnetic field. Conversely, TADF devices should exhibit a negative MEL because RISC is suppressed by the external magnetic field. Intriguingly, we observed a positive MEL in TADF devices. Moreover, the sign of the MEL was either positive or negative, and depended on experimental conditions, including doping concentration, current density and temperature. The MEL observed from our TADF devices demonstrated that ISC in the host material and RISC in the guest material coexisted. These competing processes were affected by the experimental conditions, which led to the sign change of the MEL. This work gives important insight into the energy transfer processes and the evolution of excited states in TADF devices.