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Controlling Thermally Activated Delayed Photoluminescence in CdSe Quantum Dots through Triplet Acceptor Surface Coverage.

Quantum-dot/molecule composites (QD/mol) have demonstrated useful photochemical properties for many photonic and optoelectronic applications; however, a comprehensive understanding of these materials remains elusive. This work introduces a series of cadmium(II) selenide/1-pyrenecarboxylic acid (CdSe/PCA) nanomaterials featuring bespoke PCA surface coverage on CdSe585 (coded by the peak of the first exciton absorption band) to glean insight into the QD/mol photophysical behavior. Tailoring the energy gap between the CdSe585 first exciton band (2.1 eV) and the lowest PCA triplet level (T1 = 2.0 eV) to be nearly isoenergetic, strong thermally activated delayed photoluminescence (TADPL) is observed resulting from reverse triplet-triplet energy transfer. The resultant average decay time constant (τobs) of the photoluminescence emanating from CdSe585 is deterministically controlled with surface-bound PCAn chromophores (n = average number of adsorbed PCA molecules) by shifting the triplet excited state equilibrium from the CdSe585 to the PCA molecular triplet reservoir as a function of n.