Exploring the Photophysical Origins of Bichromophoric Organic Single Crystals
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Fused-Ring Electron Acceptors (FREAs) has recently opened new possibilities in various energy and optoelectronics applications. However, their photophysical origins involving peculiar spontaneous polaron generation, proficient intersystem crossings and long-lived radiative decays remain in debate. Here, we synthesize microscale single crystals of a representative FREA, Y6, and investigate their excited state processes to uncover their structure-property relations. Synthesized via solvent diffusion, monoclinic Y6 single crystal exhibited pronounced room-temperature phosphorescence, even more significant than one with Pt-based triplet sensitizers. Temperature-dependent PL spectra further revealed thermally assisted repopulation of blue-shifted triplet state distinct from vibronic progressions. The ultrafast conversion process was explored by femtosecond transient absorption spectroscopy, which further revealed dynamic exchange interaction mediated through loosely bound excited state.