Differentiation between polaron-pair and triplet-exciton polaron spin-dependent mechanisms in organic light-emitting diodes by coherent spin beating

Pulsed electrically detected magnetic resonance offers a unique avenue to distinguish between polaron-pair (PP) and triplet-exciton polaron (TEP) spin-dependent recombination, which control the conductivity and magnetoresistivity of organic semiconductors. Which of these two fundamental processes dominates depends on carrier balance: by injecting surplus electrons we show that both processes simultaneously impact the device conductivity. The two mechanisms are distinguished by the presence of a half-field resonance, indicative of TEP interactions, and transient spin beating, the signature of PPs. Coherent spin Rabi flopping in the half-field (triplet) channel is observed, demonstrating that the triplet exciton has an ensemble phase coherence time of at least 60 ns, offering insight into the effect of carrier correlations on spin dephasing.