Haoke Zhang

Green fluorescent protein (GFP) and its derivatives have transformed biological imaging, yet fluorophores that simultaneously combine biocompatibility, structural programmability, and intrinsic long-wavelength luminescence remain scarce. Here, we develop a controllable one-pot polymerization strategy to construct nonconjugated triblock copolymers that can self-assemble into core–shell clusters. By modulating the hydrophilic–hydrophobic balance of copolymer chains, the core-to-shell ratio, chain packing, and electronic through-space interactions within the clusters can be precisely regulated, enabling tunable clusteroluminescence (CL) that extends to the deep-red and near-infrared emission region. Ultrafast spectroscopy further uncovers the excited-state dynamics of these core–shell clusters and reveals how the coupled evolution of electronic states and structures governs CL generation. Moreover, the core–shell clusters enable in vivo angiography under two-photon excitation, highlighting their potential as biocompatible nanofluorophores. These findings establish core–shell engineering as a general design principle for efficient clusteroluminogens, deepen the mechanistic understanding of CL, and pave the way for next-generation nanofluorescence technologies.

Facile and efficient transformation of inexpensive inorganic sulfides into high-value polymer materials is of great academic and industrial significance. Herein, we report a catalyst-free polyannulation strategy between potassium sulfide and internal diynes, which can efficiently produce thiophene-containing polymers (TCPs) in N,N-dimethylformamide under mild conditions. The reaction may proceed via a trisulfur radical anion-mediated mechanism, generating thiophene units in situ without the need for thiophene-containing monomers, additives, or transition metals. The resulting TCPs exhibit high molecular weights (up to 16,300 g/mol), excellent solubility and film-forming ability, and remarkable thermal stability. Their thin films display high refractive indices (n589.2 = 1.6579–1.8078) and UV-tunable optical properties. Post-oxidation transforms the polymers into aggregation-induced emission-active materials with remarkably enhanced fluorescence quantum yields in aggregate and solid states. The aggregate-state luminescent TCPs and their S,S-dioxide derivatives demonstrate organelle-specific imaging capabilities and excellent biocompatibility, highlighting their potential for advanced optical and bioimaging applications.

High‐purity emitters with a narrowband emission are a critical requirement for next‐generation displays and lighting, yet it remains a formidable challenge for purely organic materials, particularly in the pure‐violet region. Herein, a general molecular design strategy based on the “stereo‐lock” concept, represented by diarylbenzene derivatives solely from carbon and hydrogen, is presented. This strategy effectively suppresses intramolecular C─C/C─H stretching and attenuates vibronic coupling via intramolecular through‐space interactions between two aryl groups, yielding a record full width at half maximum (FWHM) of merely 6 nm at 80 K from a single molecule. In the solid state, their aggregates with intermolecular positive exciton coupling induce quantum interference that selectively quenches the v _0‐0 transition, resulting in an FWHM of 17 nm at room temperature. Leveraging this synergy, diarylbenzene‐based OLED devices with pure‐violet electroluminescence with an 18 nm FWHM and a CIE coordinate of (0.165, 0.022) are achieved. This stereo‐lock architecture circumvents the fundamental limitation of vibronic coupling in pure hydrocarbons and addresses the absence of high‐color‐purity violet OLEDs, establishing a powerful and versatile design paradigm for narrowband emitters.

High‐purity emitters with a narrowband emission are a critical requirement for next‐generation displays and lighting, yet it remains a formidable challenge for purely organic materials, particularly in the pure‐violet region. Herein, a general molecular design strategy based on the “stereo‐lock” concept, represented by diarylbenzene derivatives solely from carbon and hydrogen, is presented. This strategy effectively suppresses intramolecular C─C/C─H stretching and attenuates vibronic coupling via intramolecular through‐space interactions between two aryl groups, yielding a record full width at half maximum (FWHM) of merely 6 nm at 80 K from a single molecule. In the solid state, their aggregates with intermolecular positive exciton coupling induce quantum interference that selectively quenches the v _0‐0 transition, resulting in an FWHM of 17 nm at room temperature. Leveraging this synergy, diarylbenzene‐based OLED devices with pure‐violet electroluminescence with an 18 nm FWHM and a CIE coordinate of (0.165, 0.022) are achieved. This stereo‐lock architecture circumvents the fundamental limitation of vibronic coupling in pure hydrocarbons and addresses the absence of high‐color‐purity violet OLEDs, establishing a powerful and versatile design paradigm for narrowband emitters.

Zwitterionic hydrogels have attracted considerable attention for protein stabilization, cell encapsulation, and therapeutic delivery owing to their highly hydrated and bioinert nature. Nevertheless, developing injectable zwitterionic hydrogels that can form under mild and cytocompatible conditions remains a major challenge, especially for the delivery of fragile proteins and living cells. This challenge mainly stems from the weak intrinsic intermolecular interactions and limited reactive groups of zwitterionic polymers, which make it difficult to establish stable hydrogel networks without additional molecular modification or external crosslinking. Here, we report an injectable zwitterionic supramacromolecular hydrogel (SSH) formed by the spontaneous assembly of poly(methacryloyloxyethyl sulfobetaine) (PSBMA) and poly(styrenesulfonate) (PSSNa). Molecular dynamics simulations support the involvement of anion‐π interactions in gelation, leading to a self‐healing physically crosslinked network. SSH exhibits injectability, self‐healing behavior, intrinsic antiadhesive properties, and favorable immunocompatibility. The mild gelation process enables efficient cell encapsulation and injection while maintaining high cell viability. In addition, SSH stabilizes and delivers basic fibroblast growth factor (bFGF), resulting in improved therapeutic efficacy in a diabetic wound‐healing model. This work establishes a mild gelation strategy for injectable zwitterionic hydrogels and highlights their potential in biomedical delivery and cell‐based therapies.

We present a mechanically interlocked fluorescence switching platform that enables simultaneous, reversible control over both emission wavelength and intensity through acid/base-driven macrocycle shuttling. Our design, based on a TPE-centered rotaxane architecture, integrates pyridinium-mediated ICT and secondary ammonium recognition sites, creating an environment-sensitive fluorophore coupled to a stimuli-responsive mechanical element. This system operates via three synergistic mechanisms triggered by macrocycle translocation: modulation of the ICT state through microenvironmental polarization, enhancement of emission via confinement-induced restriction of intramolecular motion, and suppression of nonradiative decay through steric blocking of photoinduced electron transfer. By unifying structural precision with dynamic responsiveness, this strategy overcomes key limitations of conventional covalent or aggregation-based approaches and provides a generalizable blueprint for the design of programmable luminescent materials.

Room temperature phosphorescent (RTP) molecules, owing to their unique afterglow characteristics, can translate microscopic electronic transitions into macroscopic smart responses, and have gradually emerged as a research hotspot in the field of smart molecules. Benefiting from the renewability, biocompatibility, and structural tunability of cellulose, these materials provide an ideal and sustainable platform for constructing RTP systems. Significant progress has been made in this field, leading to the emergence of numerous cellulose‐based RTP material systems with novel structures and excellent performance. This review summarizes recent advances in RTP systems cellulose derivatives. First, it elucidates the underlying mechanisms of cluster‐triggered emission, followed by a detailed discussion of four key construction strategies: regulation of aggregation structures, reconstruction of clustered emission centers, hydroxyl functionalization, and host‐guest doping. In addition, innovative applications in information security and environmental monitoring are highlighted. Finally, current challenges are discussed, and perspectives on the rational design of future biomass‐based RTP materials are provided.

The development of green polymers is of critical importance for environmental sustainability and biomedical applications. Saccharides, as abundant natural polymers, have been widely used in food, agriculture, medicine, and medical devices. This review systematically summarizes the unique photophysical properties of monosaccharides, oligosaccharides, and polysaccharides that exhibit pronounced clusteroluminescence (CL). The emission mechanism based on through-space conjugation (TSC) is discussed, and negative hyperconjugation is further introduced, using polyethylene glycol as a representative structure, as an important weak interaction that modulates the electronic structures of CL materials. In addition, several unresolved issues in current CL research, extending beyond saccharide systems, are highlighted. It is anticipated that this review will stimulate further development of CL-based green polymers by advancing mechanistic understanding and enabling emerging functional applications.

Multi-axis atropisomers are ubiquitous in nature, and their intricate stereoconformations not only deepen stereochemical understanding but also elucidate fundamental principles of molecular atropisomeric dynamics. Nevertheless, insights into multi-axis atropisomerism remain limited. This work presents a systematic investigation of three classes of LaPlente-type biaxial atropisomers based on naphthalene rotors and phenyl linkers. Thermodynamically and kinetically controlled interconversion of molecular conformations is achieved in 22-NB, 11-NB, and 11-NB-8DMe. Concurrently, a direct correlation between molecular dynamics and electronic through-space conjugation (TSC) is elucidated. Furthermore, absolute separation of syn and anti conformers is accomplished in 11-NB-2DMe, whose distinct TSC-induced fluorescence enables direct visualization of dynamic conformer populations and kinetics during temporally sequential crystallization. This work provides fundamental mechanistic insights into multi-axis atropisomer stereochemistry and establishes a fluorescence-based approach as an in-situ platform for real-time analysis of molecular dynamics across life and materials sciences.