Efficient Triplet Exciton Fusion in Molecularly Doped Polymer Light‐Emitting Diodes

Abstract

probability of a triplet pair forming a singlet) in solution is >60%, much higher than the spin-statistical prediction of 25% (one pair of triplets collides to form one of the four states: one singlet S 1 and three triplets T 1 , assuming higher triplet and quintet states are inaccessible). Practical application of solar energy conversion requires the TTA-UC material to be in solid state rather than in solution phase. However, the TTA-UC quantum yield of solidstate systems remains low, typically below 5%, [10] and is moderately high (about 10%) in only one example. [19] To achieve high efficiencies, high excitation intensities (200 mW cm −2 or above) are commonly required. These imply that in solid state, the experimentally observed reaction efficiency of TTA-UC was up to about 20%, below the 25% spin-statistical limit.To achieve highly efficient triplet fusion (TTA-UC) in OLEDs and other TTA upconverters, we consider four criteria for the selection of emitters: (1) high fluorescence quantum yield, (2) short singlet lifetime, (3) long triplet lifetime, and (4) the energy of two triplet excitons, 2E(T 1 ) lies slightly above that of the singlet exciton, E(S 1 ), but below the second triplet state, E(T 2 ) (and also the energies of any spin-quintet states) (E(S 1 ) ≲ 2E(T 1 ) < E(T 2 )). The first and second criteria are prerequisites for efficient fluorescence. The third criterion is essential for the accumulation of a sufficiently high triplet population density required for rapid triplet-triplet collision processes. The fourth criterion ensures that higher-lying triplet or quintet states do not provide loss channels. The spin states of the triplet excitons give in principle nine spin configurations for the interacting triplet exciton pair, five associated with a quintet, three with a triplet, and one with the singlet state. It is generally considered that the quintet is always higher in energy than the initial triplet pair, so is neglected. If there are no energetically accessible higher-lying triplet states at E(T 2 ), we expect only the S 1 and T 1 excitons to form. Triplets produced from this reaction can be recycled and participate in a further fusion reaction. [7] The basic working principle of a triplet fusion LED (FuLED) is illustrated in Figure 1a. The initial stage (Stage I) of the device operation includes charge injection and exciton formation. Exciton formation on the emissive molecules may occur directly or indirectly through an additional exciton transfer step from a host material. If a host material is present, the S 1 and T 1 of the host are required to be higher than that of the emitter to allow efficient host-emitter energy transfer and to ensure long triplet lifetime of the emitter (Criterion 3 discussed above). The 25% singlet population can be converted to light emission (and nonradiative losses) from the singlet channel immediately, resulting in prompt electroluminescence (EL). The 75% triplet excitons remain nonemissive, but the population of triplets is When an organic light-emitting dio...

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