Design and development of multifunctional materials have drawn incredible attraction in recent years. Herein, we report the design and construction of versatile star-shaped intramolecular charge transfer (ICT)-coupled excited-state intramolecular proton transfer (ESIPT)-active mechanoresponsive and aggregation-induced emissive (AIE) luminogen triaminoguanidine-diethylaminophenol ( LH 3 ) conjugate from simple precursors triaminoguanidine hydrochloride and 4-( N , N -diethylamino)salicylaldehyde. Solvent-dependent dual emission in nonpolar to polar protic solvents implies the presence of ICT-coupled ESIPT features in the excited state. Aggregation-enhanced emissive feature of LH 3 was established in the CH 3 CN/water mixture. Furthermore, this compound exhibits mechanochromic fluorescence behavior upon external grinding. Fluorescence microscopy images of pristine, crystal, and crushed crystals confirm the naked-eye mechanoresponsive characteristics of LH 3 . In addition, LH 3 selectively sensed a Cu 2+ ion through a colorimetric and fluorescence “turn-off” route, and subsequently, the LH 3 -Cu 2+ ensemble could act as a selective and sensitive sensor for S 2– in a “turn-on” fluorescence manner via a metal displacement approach. Reversible “turn-off–turn-on” features of LH 3 with Cu 2+ /S 2– ions were efficiently demonstrated to construct the IMPLICATION logic gate function. The Cu 2+ /S 2– -responsive sensing behavior of LH 3 was established in the paper strip experiment also, which can easily be characterized by the naked eye under daylight as well as a UV lamp (λ = 365 nm).
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