Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume -, Issue -, Pages -Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.2c08479
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This study presents a series of donor-alkyl bridge-acceptor luminogens as anti-Kasha emissive molecular rotors with mechanistic insights. The origin of aggregation-induced emission and coexistence of dual fluorescence and phosphorescence are realized by suppressing Kasha's rule. Furthermore, the large energy gaps between specific states and the abundance of smaller gaps facilitate reverse intersystem crossing, resulting in thermally activated delayed fluorescence and room-temperature phosphorescence.
This work presents a series of through-space donor-alkyl bridge-acceptor (D-sigma-A) luminogens, BT2OxCz [2,2 '-(5-(3-(9H-carbazol-9-yl)-alkoxy)-1,3-phenylene)bis(benzothiazole)] (x = 3, 4, 5, and 6), as anti-Kasha emissive multifunctional molecular rotors with in-depth mechanistic insights, conveyed by experimental and theoretical results. The origin of aggregation-induced emission and coexistence of dual fluorescence and phosphorescence are realized from hot excitons (especially from the bright emissive states of S7/S5 and T3) by suppressing Kasha's rule. More importantly, the large energy gaps (LEST) between S7/S5 and S1 states (T3 and T1 states) along with an abundance of small LEST between singlet charge transfer and triplet locally excited states facilitate reverse intersystem crossing resulting in thermally activated delayed fluorescence and room-temperature phosphor-escence simultaneously. Besides, alkyl chain length-induced distinct H-and J-aggregation offers tunable triplet-harvesting behavior and white-light emission along with two different reversible mechanoresponsive properties viz. mechanoluminescence and mechanochromism, respectively.
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