Abstract
A combined theoretical and experimental investigation into the role of concerted long- (dipole coupling) and short-range (orbital overlap mediated excimer) electronic interactions in modulating the emission of six crystalline acetylanthracenes (1-3) is reported. Friedel-Crafts acylation of anthracene rendered crystalline acetylanthracenes with discrete close packing, varied orbital overlap, and resultant distinct emission (blue-green-yellow) from cooperative excimer and dipole coupling. Time-resolved emission spectroscopy (TRES) studies and the Kasha's exciton theory based quantitative estimation of dipole coupling (mean-field approximation) substantiates the exciton dynamics in crystalline 1-3. Extension of the Kasha's exciton model beyond the traditional nearest-neighbor approach, and consistent agreement among the computed spectral shifts and TRES temporal components, corroborate a holistic approach to decipher the exciton relaxation dynamics in the molecular assembly of novel photonic materials.
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