We have designed a series of pentacene dimers separated by homoconjugated or nonconjugated bridges that exhibit fast and efficient intramolecular singlet exciton fission (iSF). These materials are distinctive among reported iSF compounds because they exist in the unexplored regime of close spatial proximity but weak electronic coupling between the singlet exciton and triplet pair states. Using transient absorption spectroscopy to investigate photophysics in these molecules, we find that homoconjugated dimers display desirable excited-state dynamics, with significantly reduced recombination rates as compared to conjugated dimers with similar singlet fission rates. In addition, unlike conjugated dimers, the time constants for singlet fission are relatively insensitive to the interplanar angle between chromophores, since rotation about σ bonds negligibly affects the orbital overlap within the π-bonding network. In the nonconjugated dimer, where the iSF occurs with a time constant >10 ns, comparable to the fluorescence lifetime, we used electron spin resonance spectroscopy to unequivocally establish the formation of triplet-triplet multiexcitons and uncoupled triplet excitons through singlet fission. Together, these studies enable us to articulate the role of the conjugation motif in iSF.

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A solution-based fabrication of fl exible and light-weight light-emitting devices on paper substrates is reported. Two different types of paper substrates are coated with a surface-emitting light-emitting electrochemical cell (LEC) device: a multilayer-coated specialty paper with an intermediate surface roughness of 0.4 µm and a low-end and low-cost copy paper with a large surface roughness of 5 µm. The entire device fabrication is executed using a handheld airbrush, and it is notable that all of the constituent layers are deposited from solution under ambient air. The top-emitting paper-LECs are highly fl exible, and display a uniform light emission with a luminance of 200 cd m −2 at a current conversion effi cacy of 1.4 cd A −1 .

Light-emitting electrochemical cells, featuring uniform and efficient light emission over areas of 200 cm(2) , are fabricated under ambient air with a for-the-purpose developed "spray-sintering" process. This fault-tolerant fabrication technique can also produce multicolored emission patterns via sequential deposition of different inks based on identical solvents. Significantly, additive spray-sintering using a mobile airbrush allows a straightforward addition of emissive function onto a wide variety of complex-shaped surfaces, as exemplified by the realization of a light-emitting kitchenware fork.