Metal-free organic phosphorescence materials are of imperious demands in optoelectronics and bioelectronics. However, it is still a formidable challenge to develop a material with simultaneous efficiency and lifetime enhancement under ambient conditions. In this study, we design and synthesize a new class of high efficient ultralong organic phosphorescence (UOP) materials through self-assembly of melamine and aromatic acids in aqueous media. A supramolecular framework can be formed via multiple intermolecular interactions, building a rigid environment to lock the molecules firmly in a three-dimensional network, which not only effectively limits the nonradiative decay of the triplet excitons but also promotes the intersystem crossing. Thus, the supermolecules we designed synchronously achieve an ultralong emission lifetime of up to 1.91 s and a high phosphorescence quantum efficiency of 24.3% under ambient conditions. To the best of our knowledge, this is the best performance of UOP materials with simultaneous efficiency and lifetime enhancement. Furthermore, it is successfully applied in a barcode identification in darkness. This result not only paves the way toward high efficient UOP materials but also expands their applications.
Smart materials with ultralong phosphorescence are rarely investigated and reported. Herein we report on a series of molecules with unique dynamic ultralong organic phosphorescence (UOP) features, enabled by manipulating intermolecular interactions through UV light irradiation. Our experimental data reveal that prolonged irradiation of single-component organic phosphors of PCzT, BCzT, and FCzT under ambient conditions can activate UOP with emission lifetimes spanning from 1.8 to 1330 ms. These phosphors can also be deactivated back to their original states with short-lived phosphorescence by UV irradiation for 3 h at room temperature or through thermal treatment. Additionally, the dynamic UOP was applied successfully for a visual anti-counterfeiting application. These findings may provide unique insight into dynamic molecular motion for optical processing and expand the scope of smart-response materials for broader applications.
Ultralong organic phosphorescence (UOP) based on metal-free porous materials is rarely reported owing to rapid nonradiative transition under ambient conditions. In this study, hydrogen-bonded organic aromatic frameworks (HOAFs) with different pore sizes were constructed through strong intralayer π-π interactions to enable ultralong phosphorescence in metal-free porous materials under ambient conditions for the first time. Impressively, yellow UOP with a lifetime of 79.8 ms observed for PhTCz-1 lasted for several seconds upon ceasing the excitation. For PhTCz-2 and PhTCz-3, on account of oxygen-dependent phosphorescence quenching, UOP could only be visualized in N , thus demonstrating the potential of phosphorescent porous materials for oxygen sensing. This result not only outlines a principle for the design of new HOFs with high thermal stability, but also expands the scope of metal-free luminescent materials with the property of UOP.
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