Chemical systems with external control capability and selfrecoverability are promising since they can avoid additional chemical or energy imposition during the working process. However, it remains challenging to employ such a nonequilibrium method for the engineering of optoelectronic function and for visualization. Here, we report a functional molecule that can undergo intense conformational regulation upon photoexcitation. It enables a dynamical change in hydrophobicity and a follow-up molecular aggregation in aqueous media, accordingly leading to an aggregation-induced phosphorescence (AIP) behavior. This successive performance is self-recoverable, allowing a rapid (second-scale cycle) and long-standing (>10 3 cycles) flicker ability under rhythmical control of the AIP. Compared with traditional bidirectional manipulations, such monodirectional photocontrol with spontaneous reset profoundly enhances the operability while mostly avoiding possible side reactions and fatigue accumulation. Furthermore, this material can serve as a type of luminescent probe for dynamically strengthening visualization in bioimaging.A rtificial molecular switches continue to attract research attention due to their fascinating structures and smart control performances (1-5). Nevertheless, most of these chemical systems work between two or more stable states, and the rest of them requires at least a secondary chemical or energy stimuli, imposing additional inconvenience and the possibility of doubling fatigue accumulation (6-8). Inspired by the underlying mechanism of functional natural systems, scientists began to design and develop molecules with self-recoverability for nonequilibrium action control (9-11). Among the control methods, photocontrol is still a superior fashion because light stimuli are usually rapid and precise, and can be operated remotely (12,13). In contrast to well-studied photochemical processes like photoreaction, photocyclization, and photoisomerization (14, 15), a photocontrol approach with selfrecoverability largely connects to a photoexcitation principle. Thus, it may generally suffer from ultrafast energy relaxation and dissipation, and is extremely difficult to be utilized in materials. Engineering of optoelectronic function and visualization via such a photocontrol method is particularly challenging but also desirable.While luminescent probe techniques enabled a significant scientific advancement in visualized analysis, sensing, and imaging (16)(17)(18), in this work, we expect to impose a photocontrol with self-recoverability into the advancing of operating methods for molecular luminescence. Aggregation-induced emission (AIE) is a type of approach where the molecules can exhibit high luminescence in condensed or constraint states by overcoming the aggregation-caused quenching effect (19)(20)(21). Controllable AIE probes that utilize specific chemical reactions have emerged to facilitate a series of frontier biological usage (22)(23)(24)(25). In contrast, the necessity of spontaneous, repeatable, and rhyth...
Developing molecules with high emission efficiency both in solution and the solid state is still a great challenge, since most organic luminogens are either aggregation‐caused quenching or aggregation‐induced emission molecules. This dilemma was overcome by integrating planar and distorted structures with long alkyl side chains to achieve DAπAD type emitters. A linear diphenyl–diacetylene core and the charge transfer effect ensure considerable planarity of these molecules in the excited state, allowing strong emission in dilute solution (quantum yield up to 98.2 %). On the other hand, intermolecular interactions of two distorted cyanostilbene units restrict molecular vibration and rotation, and long alkyl chains reduce the quenching effect of the π–π stacking to the excimer, eventually leading to strong emission in the solid state (quantum yield up to 60.7 %).
Enantiodifferentiation is crucial in organic chemistry, pharmacochemistry, material chemistry, and life science. However, it remains tremendously challenging to achieve a broad enantioselectivity to different types of chiral substrates via a single-material design. Here, we report a coassembled organogel strategy with chirality transfer to make an enantioselective generality possible. This coassembly contains two components: a chiral rigid molecular linker and an achiral block copolymer. Different from routine helically packed chiral self-assemblies, chirality transfer from the linker to the copolymer directed the coassembly to form a phase-segregated twisted nanofiber, in cooperation with H-bonding and microphase segregation. An organogel was accordingly formed by the further crosslinking in ethanol, where the rigid chiral linker served as the scaffold. On this basis, the system becomes highly sensitive, enabling a naked-eye sensing toward the single enantiomer of a diverse series of chiral species (including axial, point, planar, and polymeric chirality) via gel-to-micelle transformation, due to the asymmetric interaction hampering the chirality transfer in the coassembly and destroying the hierarchical structure. Such a strategy, based on a significant amplification of the stereoselective interactions, facilitates a simple and straightforward way to distinguish a broad optical activity independent of devices.
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