Achieving multicolor,precisely tunable cluster-induced emission in nonconjugated polymers remains a considerable challenge.Herein,we present a generalizable and scalable methodology for fabricating monodisperse,color-...Achieving multicolor,precisely tunable cluster-induced emission in nonconjugated polymers remains a considerable challenge.Herein,we present a generalizable and scalable methodology for fabricating monodisperse,color-tunable clusteroluminescence(CL)microspheres,enabling multimodal color tuning across the spectrum from blue to orange-red through precise control of monomer type and ratio,sulfonation time,and pH conditions.Density functional theory(DFT)simulations demonstrate that conformational rigidity,resulting from the synergistic combination of prevalent hydrogen-bonding interactions,short interatomic contacts,and oxygen cluster formation,significantly enhances emission efficiency,leading to dual broadband visible emissions across the 400–700 nm wavelength range.The optimized sulfonated poly(divinylbenzene-styrene-methyl methacrylate)microspheres with 30%methyl methacrylate(MMA)content(SPSMMAs-30)exhibit excellent monodispersity and strong fluorescence across 13 standard channels of flow cytometry,with fluorescence coefficient of variation(CV)values consistently below 3%,fulfilling requirements for routine flow cytometer calibration.Compared with commercial calibration microspheres,SPSMMAs-30 show significantly higher photobleaching resistance and long-term environmental stability.Significantly,this protocol enables the first kilogram-scale synthesis of CLmicrospheres with highly reproducible optical properties.Furthermore,SPSMMAs-30 demonstrate sensitive tetracycline detection and promising performance in multicolor anticounterfeiting applications,substantially broadening the scope of nonconjugated CL materials for biomedicine,diagnostics,and materials science.展开更多
Self-assembled inorganic halide perovskite superlattices(HPSLs)have attracted extensive attention for their well-ordered structure and unique collective photonic properties,which differ from those of individual nanocr...Self-assembled inorganic halide perovskite superlattices(HPSLs)have attracted extensive attention for their well-ordered structure and unique collective photonic properties,which differ from those of individual nanocrystals(NCs).However,the manipulation of ordered HPSLs with all-halogen and alloyed halogen components,as well as the regulation of their coherent spontaneous emission across the visible spectrum,remains underexplored.In this study,we employ a combination of anion-exchange reactions and a slow solvent evaporation strategy to self-assemble monodisperse,uniform all inorganic perovskite NCs into a series of well-defined,long-range ordered,and densely packed CsPbX3(X=Cl,Br,I,and mixed halide systems such as Cl/Br,Br/I,and Cl/Br/I)superlattices,achieving coherent photoluminescence(PL)emission across the entire visible spectrum(400–700 nm).Notably,the collective coherent emission of all HPSLs exhibits dynamic redshifts and accelerated collective radiative decay due to strong electronic coupling between NCs at cryogenic temperatures(7 K).This study not only systematically investigates all-halide compositional HPSLs but also paves the way for quantum light source applications across the visible spectrum.展开更多
基金supported by the Ministry of Science and Technology of the People’s Republic of China(no.2022YFC2406600)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(no.Y2023088)the Innovative Key Project of Suzhou Institute of Biomedical Engineering and Technology,the Chinese Academy of Sciences(no.CX202501001).
文摘Achieving multicolor,precisely tunable cluster-induced emission in nonconjugated polymers remains a considerable challenge.Herein,we present a generalizable and scalable methodology for fabricating monodisperse,color-tunable clusteroluminescence(CL)microspheres,enabling multimodal color tuning across the spectrum from blue to orange-red through precise control of monomer type and ratio,sulfonation time,and pH conditions.Density functional theory(DFT)simulations demonstrate that conformational rigidity,resulting from the synergistic combination of prevalent hydrogen-bonding interactions,short interatomic contacts,and oxygen cluster formation,significantly enhances emission efficiency,leading to dual broadband visible emissions across the 400–700 nm wavelength range.The optimized sulfonated poly(divinylbenzene-styrene-methyl methacrylate)microspheres with 30%methyl methacrylate(MMA)content(SPSMMAs-30)exhibit excellent monodispersity and strong fluorescence across 13 standard channels of flow cytometry,with fluorescence coefficient of variation(CV)values consistently below 3%,fulfilling requirements for routine flow cytometer calibration.Compared with commercial calibration microspheres,SPSMMAs-30 show significantly higher photobleaching resistance and long-term environmental stability.Significantly,this protocol enables the first kilogram-scale synthesis of CLmicrospheres with highly reproducible optical properties.Furthermore,SPSMMAs-30 demonstrate sensitive tetracycline detection and promising performance in multicolor anticounterfeiting applications,substantially broadening the scope of nonconjugated CL materials for biomedicine,diagnostics,and materials science.
基金financially supported by the National Natural Science Foundation of China(52072281)the Major Program of the National Natural Science Foundation of China(22293021)+1 种基金the Wuhan University of Technology Doctoral Research Initiation Fee(40120543)the Hubei Province's State-allocated Dual-class Research Platform Fee(40120623).
文摘Self-assembled inorganic halide perovskite superlattices(HPSLs)have attracted extensive attention for their well-ordered structure and unique collective photonic properties,which differ from those of individual nanocrystals(NCs).However,the manipulation of ordered HPSLs with all-halogen and alloyed halogen components,as well as the regulation of their coherent spontaneous emission across the visible spectrum,remains underexplored.In this study,we employ a combination of anion-exchange reactions and a slow solvent evaporation strategy to self-assemble monodisperse,uniform all inorganic perovskite NCs into a series of well-defined,long-range ordered,and densely packed CsPbX3(X=Cl,Br,I,and mixed halide systems such as Cl/Br,Br/I,and Cl/Br/I)superlattices,achieving coherent photoluminescence(PL)emission across the entire visible spectrum(400–700 nm).Notably,the collective coherent emission of all HPSLs exhibits dynamic redshifts and accelerated collective radiative decay due to strong electronic coupling between NCs at cryogenic temperatures(7 K).This study not only systematically investigates all-halide compositional HPSLs but also paves the way for quantum light source applications across the visible spectrum.
