Polymer-based room-temperature phosphorescence (RTP) materials with high flexibility and large-area producibility are highly promising for applications in organic electronics. However, achieving such photophysical materials is challenging because of difficulties in populating and stabilizing susceptible triplet excited states at room temperature. Herein large-area, flexible, transparent, and long-lived RTP systems prepared by doping rationally selected organic chromophores in a poly(vinyl alcohol) (PVA) matrix were realized through a hydrogen-bonding and coassembly strategy. In particular, the 3,6-diphenyl-9H-carbazole (DPCz)-doped PVA film shows long-lived phosphorescence emission (up to 2044.86 ms) and a remarkable duration of afterglow (over 20 s) under ambient conditions. Meanwhile, the 7H-dibenzo[c,g]carbazole (DBCz)-doped PVA film exhibits high absolute luminance of 158.4 mcd m2 after the ultraviolet excitation source is removed. The RTP results not only from suppressing the nonradiative decay by abundant hydrogen-bonding interactions in the PVA matrix but also from minimizing the energy gap (ΔE ST) between the singlet state and the triplet state through the coassembly effect. On account of the outstanding mechanical properties and the afterglow performance of these RTP materials, they were applied in the fabrication of flexible 3D objects with repeatable folding and curling properties. Importantly, the multichannel afterglow light-emitting diode arrays were established under ambient conditions. The present long-lived phosphorescent systems demonstrate a bright opportunity for the production of large-area, flexible, and transparent emitting materials.
Organic long‐persistent luminescence (OLPL) materials have attracted wide attention on account of their fascinating luminescence properties, presenting application prospects in the fields of bioimaging, information security, displays, anti‐counterfeiting, and so on. Some effective strategies have been developed to promote the intersystem crossing (ISC) of the excited singlet state to triplet state and limit nonradiative transition, and thus OLPL materials with long lifetime (more than 1s) and high quantum yield have been explored. However, OLPL materials with dynamic and excitation‐dependent characteristics are rarely reported. In this work, two novel polyphosphazene derivatives containing carbazolyl units are designed and synthesized successfully, and then they are doped into poly(vinyl alcohol) (PVA) films to achieve polymeric long‐persistent luminescence (PLPL). Unexpectedly, excitation‐dependent PLPL (ED‐PLPL) is obtained under ambient conditions (in air at room temperature), and the persistent luminescence color can be changed from blue to green upon varying the excitation wavelength. At the same time, a dynamic cycle of ED‐PLPL is realized based on the formation and destruction of hydrogen bonding interactions between the PVA chains and polyphosphazene phosphor. This work provides a new strategy for the design of color‐tunable polymeric luminescent materials under ambient conditions.
While manipulating the helicity of nanostructures is a challenging task, it attracts great research interest on account of its crucial role in better understanding the formation mechanisms of helical systems. For the supramolecular chirality in self-assembly systems, one challenge is how to understand the origin of supramolecular chirality and inherent helicity information on nanostructures regulated by functionality-oriented stacking modes (such as J- and H-aggregation) of building blocks. Herein, two-component hydrogels were prepared by phenylalanine-based enantiomers and achiral bis(pyridinyl) derivatives, where helical nanofibers with inverse handedness as well as controllable helical pitch and diameter were readily obtained through stoichiometric coassembly of these building blocks. The helix inversion was achieved by the transition between the J- and H-aggregation of bis(pyridinyl) derivatives, which was collectively confirmed by circular dichroism, scanning electron microscopy, Fourier transform infrared spectroscopy, and single X-ray crystallography. Interestingly, the helical coassemblies with opposite handedness could be obtained not only from the enantiomeric building blocks but also from the chiral monomers with the same configurational chirality by exchanging achiral additives. This work provides insight into the origin and helicity inversion of supramolecular chirality in molecular self-assembly systems and may shine light on the precise fabrication of chiral nanostructures for potential applications in smart display devices, optoelectronics, and biological systems.
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