Bay-site carboxyl functionalized perylene diimide derivative 1,7-COOH-PDI-C_(12)(PDI-COOH)was synthesized and distinct enhanced fluorescence was observed through combining with calcium ion(Ca^(2+))in THF/H_(2)O soluti...Bay-site carboxyl functionalized perylene diimide derivative 1,7-COOH-PDI-C_(12)(PDI-COOH)was synthesized and distinct enhanced fluorescence was observed through combining with calcium ion(Ca^(2+))in THF/H_(2)O solution.The assembly and fluorescence behavior of PDI-COOH/Ca^(2+)were studied in detail by changing hydration state with different concentrations.Based on the differences in assembly morphology and stoichiometric ratios of PDICOOH/Ca^(2+),we proposed the fluorescence emission mechanism of PDI-COOH/Ca^(2+)in THF/H_(2)O and THF,respectively.This work reveals a novel strategy of aggregated state fluorescence enhancement and reminds us of the important role of water in molecular fluorescence emission and assembly.展开更多
Silver ion(Ag^(+))is a highly toxic metal ion,and its monitoring in water or food resources has become extraordinarily necessary within the scope of human health.In the light of the fact of Ag^(+)-induced folding stru...Silver ion(Ag^(+))is a highly toxic metal ion,and its monitoring in water or food resources has become extraordinarily necessary within the scope of human health.In the light of the fact of Ag^(+)-induced folding structure of specific peptides,an unlabeled and highselectivity Ag^(+)assay is presented by means of intrinsic fluorescence of peptides.Under the quenching effect of gold nanoparticles(AuNPs),characteristic fluorescence of peptides could be considerably reduced by rapid modification.Along with the Ag adding,the fluorescence signals of peptide-AuNPs are largely enhanced by the behavior between peptides and Agt.This is basically involving the formation of 4-coordinated complexes,generating the changes of peptides in structure and fluorescence properties.Under this circumstance,the adverse influence of plenty of interfering ions is suppressed,including the toxic Hg^(2+),Pb^(2+).The results highlight that Ag ions could be selectively recognized as low as 2.4 nmol/L with a linear range of 5 to 800 nmol/L.In comparison with other programs,the given approach declares simplicity,sensitivity,and superior selectivity.Furthermore,the biosensor excels in the practical application in water samples(e.g.,lake,tap and drinking water)owing to its non-interference and on-site rapid determination.展开更多
Perylene diimide(PDI)derivatives have emerged as a class of important organic fluorescent materials owing to their high extinction coefficient,excellent thermal and photostability,and versatile structural tunability.H...Perylene diimide(PDI)derivatives have emerged as a class of important organic fluorescent materials owing to their high extinction coefficient,excellent thermal and photostability,and versatile structural tunability.However,due to its intrinsic rigid planar structure,π-πstacking is easy to occur,resulting in aggregation-caused quenching(ACQ).In recent years,extensive efforts have been devoted to overcome this challenge and enhance the fluorescence performance of PDIs.This review systematically summarizes representative strategies from three major perspectives:(i)Rational molecular design,including the introduction of bulky aromatic substituents,dendritic or polyhedral oligomeric silsesquioxane(POSS)units to provide steric hindrance,as well as the activation of aggregation-induced emission(AIE);(ii)Polymer-based regulation strategies,including physical blending with polymer hosts and covalent integration into polymer backbones,which provide spatial isolation and structural robustness;and(iii)Supramolecular assembly,where host-vip inclusion and self-assembly pathways precisely tune intermolecular packing and excitonic coupling.These strategies have enabled significant improvements in fluorescence quantum yield(FLQY)across solution,aggregate,and solid states.Furthermore,highly emissive perylene diimide(PDI)derivatives have demonstrated broad applicability in biomedicine,sensing and anti-counterfeiting,and optoelectronic devices such as organic light-emitting diodes(OLEDs).This review highlights the fundamental design principles,performance optimization strategies,and emerging application frontiers of PDI-based luminescent materials,providing guidance for their further development toward multifunctional and sustainable optoelectronic technologies.展开更多
Most of acridine based thermally activated delayed fluorescence(TADF)emitters are characterized by advantageous reverse intersystem crossing(RISC)rate(kRISCs)due to the perpendicular orientation of the acridine donor ...Most of acridine based thermally activated delayed fluorescence(TADF)emitters are characterized by advantageous reverse intersystem crossing(RISC)rate(kRISCs)due to the perpendicular orientation of the acridine donor to the acceptor moiety,but suffer from a poor radiation rate(kr)typically in the order of 10^(6) s^(−1).Herein,two sky blue TADF emitters 3,6-DMAC-AD-Py and 3,6-SFAC-AD-Py were developed by linking acridine(DMAC)and spiro-fluorene-acridine(SFAC)donors to 10-(pyridin-2-yl)acridin-9(10H)-one(AD-Py)acceptor.Larger SFAC and electron-deficient pyridyl groups are deliberately incorporated in 3,6-SFACAD-Py since the unique through-space interaction between them is designed to drive the rotation of inner acridine ring in SFAC for enhancing frontier molecular orbitals overlap while keeping a decent TADF behavior.Thus,the kr of 3,6-SFACAD-Py is increased to 1.5×10^(7) s^(−1).Simultaneously,SFAC donors improve spin orbital coupling strength and reduce the energy gaps,generating kRISC of 1.8×10^(6) s^(−1).This is the first acridine donor based TADF emitter realizing kr of 10^(7) s^(−1) and kRISC of 10^(6) s^(−1) by a through-space interaction strategy.3,6-SFACAD-Py enables a highly efficient sky-blue organic light-emitting diode with a maximum external quantum efficiency(EQE)of 34.7%and Commission International de I'Eclairage coordinates of(0.19,0.37).More importantly,the EQE still remained 27.6%and 16.9%at high brightness of 1000 and 10,000 cd m^(−2).展开更多
Over the past ten years,numerous papers have been published on the use of indocyanine green(ICG)fluorescence in liver surgery for hepatocellular carcinoma(HCC).There are many different applications.The first involves ...Over the past ten years,numerous papers have been published on the use of indocyanine green(ICG)fluorescence in liver surgery for hepatocellular carcinoma(HCC).There are many different applications.The first involves targeting superficial tumors in patients with macronodular cirrhosis and an irregular liver surface.In a minimally invasive setting,the lack of tactile feedback on the hepatic surface makes detecting subcapsular HCC with ultrasound alone challenging.ICG fusion images can mimic the tactile feedback of the hand and act as an ultrasound booster.ICG fluorescence can be used to evaluate tumor residues after minimally invasive thermal ablation.ICG fluorescence imaging can also be used to identify the grade of HCC early on and evaluate the microinvasive component.展开更多
Images taken in dim environments frequently exhibit issues like insufficient brightness,noise,color shifts,and loss of detail.These problems pose significant challenges to dark image enhancement tasks.Current approach...Images taken in dim environments frequently exhibit issues like insufficient brightness,noise,color shifts,and loss of detail.These problems pose significant challenges to dark image enhancement tasks.Current approaches,while effective in global illumination modeling,often struggle to simultaneously suppress noise and preserve structural details,especially under heterogeneous lighting.Furthermore,misalignment between luminance and color channels introduces additional challenges to accurate enhancement.In response to the aforementioned difficulties,we introduce a single-stage framework,M2ATNet,using the multi-scale multi-attention and Transformer architecture.First,to address the problems of texture blurring and residual noise,we design a multi-scale multi-attention denoising module(MMAD),which is applied separately to the luminance and color channels to enhance the structural and texture modeling capabilities.Secondly,to solve the non-alignment problem of the luminance and color channels,we introduce the multi-channel feature fusion Transformer(CFFT)module,which effectively recovers the dark details and corrects the color shifts through cross-channel alignment and deep feature interaction.To guide the model to learn more stably and efficiently,we also fuse multiple types of loss functions to form a hybrid loss term.We extensively evaluate the proposed method on various standard datasets,including LOL-v1,LOL-v2,DICM,LIME,and NPE.Evaluation in terms of numerical metrics and visual quality demonstrate that M2ATNet consistently outperforms existing advanced approaches.Ablation studies further confirm the critical roles played by the MMAD and CFFT modules to detail preservation and visual fidelity under challenging illumination-deficient environments.展开更多
MnO_(x)-CeO_(2)catalysts for the low-temperature selective catalytic reduction(SCR)of NO remain vulnerable to water and sulfur poisoning,limting their practical applications.Herein,we report a hydrophobic-modified MnO...MnO_(x)-CeO_(2)catalysts for the low-temperature selective catalytic reduction(SCR)of NO remain vulnerable to water and sulfur poisoning,limting their practical applications.Herein,we report a hydrophobic-modified MnO_(x)-CeO_(2)catalyst that achieves enhanced NO conversion rate and stability under harsh conditions.The catalyst was synthesized by decorating MnOx crystals with amorphous CeO_(2),followed by loading hydrophobic silica on the external surfaces.The hydrophobic silica allowed the adsorption of NH_(3)and NO and diffusion of H,suppressed the adsorption of H_(2)O,and prevented SO_(2)interaction with the Mn active sites,achieving selective molecular discrimination at the catalyst surface.At 120℃,under H_(2)O and SO_(2)exposure,the optimal hydrophobic catalyst maintains 82%NO conversion rate compared with 69%for the unmodified catalyst.The average adsorption energies of NH_(3),H_(2)O,and SO_(2)decreased by 0.05,0.43,and 0.52 eV,respectively.The NO reduction pathway follows the Eley-Rideal mechanism,NH_(3)^(*)+*→NH_(2)^(*)+H^(*)followed by NH_(2)^(*)+NO^(*)→N_(2)^(*)+H_(2)O^(*),with NH_(3)dehydrogenation being the rate determining step.Hydrophobic modification increased the activation energy for H atom transfer,leading to a minor decrease in the NO conversion rate at 120℃.This work demonstrates a viable strategy for developing robust NH_(3)-S CR catalysts capable of efficient operation in water-and sulfur-rich environments.展开更多
Two-dimensional(2D)MoS_(2) is considered an excellent candidate material for nextgeneration photodetectors.However,the high dark current and low photocurrent in MoS_(2) devices severely hinder their practical applicat...Two-dimensional(2D)MoS_(2) is considered an excellent candidate material for nextgeneration photodetectors.However,the high dark current and low photocurrent in MoS_(2) devices severely hinder their practical application.Strategies for suppressing dark current and enhancing photocurrent should be explored.Herein,we propose a modification strategy for MoS_(2) by utilizing Ag_(70) nanoclusters(NCs)as electron reservoirs and photoabsorbers to suppress dark current and enhance the photocurrent of 2D MoS_(2) photodetector.Remarkably,the dark current is effectively suppressed by four orders of magnitude,while the photocurrent is enhanced by over tenfold upon modification with Ag_(70) NCs,compared to the pristine MoS_(2) photodetector.The reduction in dark current is attributed to charge transfer from MoS_(2) to Ag_(70) NCs owing to the strong electronwithdrawing property of Ag_(70) NCs.The increase in photocurrent benefits from enhanced optical absorption of the photodetector after Ag_(70) NCs modification and the subsequent injection of photoexcited electrons from Ag_(70) NCs to MoS_(2).Compared to isolated MoS_(2),the modulated photodetector shows exceptional improvements in several key figures of merit(such as responsivity,detectivity,external quantum efficiency,and photoswitching on/off ratio).This study opens up new avenues for building high-performance 2D MoS_(2) photodetectors.展开更多
Lateral movement represents the most covert and critical phase of Advanced Persistent Threats(APTs),and its detection still faces two primary challenges:sample scarcity and“cold start”of new entities.To address thes...Lateral movement represents the most covert and critical phase of Advanced Persistent Threats(APTs),and its detection still faces two primary challenges:sample scarcity and“cold start”of new entities.To address these challenges,we propose an Uncertainty-Driven Graph Embedding-Enhanced Lateral Movement Detection framework(UGEA-LMD).First,the framework employs event-level incremental encoding on a continuous-time graph to capture fine-grained behavioral evolution,enabling newly appearing nodes to retain temporal contextual awareness even in the absence of historical interactions and thereby fundamentally mitigating the cold-start problem.Second,in the embedding space,we model the dependency structure among feature dimensions using a Gaussian copula to quantify the uncertainty distribution,and generate augmented samples with consistent structural and semantic properties through adaptive sampling,thus expanding the representation space of sparse samples and enhancing the model’s generalization under sparse sample conditions.Unlike static graph methods that cannot model temporal dependencies or data augmentation techniques that depend on predefined structures,UGEA-LMD offers both superior temporaldynamic modeling and structural generalization.Experimental results on the large-scale LANL log dataset demonstrate that,under the transductive setting,UGEA-LMD achieves an AUC of 0.9254;even when 10%of nodes or edges are withheld during training,UGEA-LMD significantly outperforms baseline methods on metrics such as recall and AUC,confirming its robustness and generalization capability in sparse-sample and cold-start scenarios.展开更多
Monodisperse Ag nanoparticles with diameters of about 3.4 nm were synthesized by a facile ultrasonic synthetic route at room temperature with the reduction of borane-tert-butylamine in the presence of oleylamine (OAm...Monodisperse Ag nanoparticles with diameters of about 3.4 nm were synthesized by a facile ultrasonic synthetic route at room temperature with the reduction of borane-tert-butylamine in the presence of oleylamine (OAm) and oleic acid (OA). The reaction parameters of time, the molar ratios of OAm to OA were studied, and it was found that these parameters played important roles in the morphology and size of the products. Meanwhile, surface enhanced Raman spectrum (SERS) property suggested the Ag nanoparticles exhibited high SERS effect on the model molecule Rhodamine 6G. And also, two-photon fluorescence images showed that the silver nanoparticles had high performances in fluorescence enhancement.展开更多
A series of fluorescent chemosensors 1-3 were synthesized to detect transition metal ions. At the room temperature, fluorescence intensities of these chemosensors in acetonitrile without transition metal ions were fou...A series of fluorescent chemosensors 1-3 were synthesized to detect transition metal ions. At the room temperature, fluorescence intensities of these chemosensors in acetonitrile without transition metal ions were found to be very weak, due to the process of the efficient intramolecular photoinduced electron transfer (PET). However, after addition of the transition metal ions, the chemoscnsor 1-3 exhibits obvious fluorescence enhancement. Moreover, the intensity of the fluorescence emission of chemosensors increases significantly in the presence of Zn^2+ and Cd^2+. The fluorescent chemosensors with different polyamine as receptors show diverse affinity abilities to the transition metal ions and signal the receptor-metal ion interaction by the intensity change of fluorescence emission.展开更多
A novel fluorescent aqueous polyurethane emulsion DDAQ-TDI-PU was synthesized by blocking the anthraquinone moiety of 1,4-diamino-2,3-diphenoxyanthraquinone(DDAQ) into polyurethane chain using 2,4-tolylene diisocyan...A novel fluorescent aqueous polyurethane emulsion DDAQ-TDI-PU was synthesized by blocking the anthraquinone moiety of 1,4-diamino-2,3-diphenoxyanthraquinone(DDAQ) into polyurethane chain using 2,4-tolylene diisocyanate(TDI),poly(propylene glycol) and 2,2-dimethylol propionic acid.The chain structure of DDAQ-TDI-PU was confirmed by means of Fourier transform infrared spectroscopy and UV-vis analysis.Comparing to the UV-vis spectrum of DDAQ,DDAQ-TDI-PU showed a hypsochromic shift from the absorption maxima of 518,558,609 nm to 510,548,586 nm,respectively.It was found that the fluorescence intensity of DDAQ-TDI-PU emulsion was enhanced greatly comparing with that of DDAQ.The fluorescence of DDAQ-TDI-PU was very stable not only for the long term storage but also for the fluorescence quencher.展开更多
The fluorescence of terbium (Ⅲ) was enhanced by about three orders of magnitude in the presence of trimellitic acid (benzene-1, 2, 4-tricarboxylic acid (TLA)) in aqueous solution at pH 6. The fluorescence inten...The fluorescence of terbium (Ⅲ) was enhanced by about three orders of magnitude in the presence of trimellitic acid (benzene-1, 2, 4-tricarboxylic acid (TLA)) in aqueous solution at pH 6. The fluorescence intensity could be greatly increased when the system of Tb^3+-TLA was treated with La^3+ (or Gd^3+) and TritonX- 100. The addition of La^3+ (or Gd^3+) enhanees the fluorescence of the system by about two orders of magnitude due to cofluorescenee, and the TritonX-100 micellar medium plays an important role for stabilization of the system. Both the intermolecular energy transfer mode and intramolecular energy transfer mode are responsible for the mechanism of fluorescence enhancement. In the optimum condi- tions, the fluorescence intensity is a linear function of Tb3~ concentration in the range of 7.8 × 10^-9-3.6 × 10^4 mol/L for the system Tb^3+-La^3+-TLA and 1.0 × 10^-8-4.7 × 10^-5 mol/L for the system Tb^3+-Gd^3+-TLA, and the limits of detection are 4.6 × 10^-10 mol/L and 6.0 × 10^-10 mol/L, respectively.展开更多
A new substrate,aligned Ag nanowires decorated with silver nanoparticle composite structure(AgNWs@AgNPs),was fabricated to investigate metalenhanced fluorescence(MEF) and its mechanism.The new composite structure was ...A new substrate,aligned Ag nanowires decorated with silver nanoparticle composite structure(AgNWs@AgNPs),was fabricated to investigate metalenhanced fluorescence(MEF) and its mechanism.The new composite structure was fabricated via a three-phase interface assembly method followed by SnCl2 sensitization and AgNO3 reduction process.The size and distribution of the nanoparticles on silver nanowires increased with the sensitization and reduction cycles.The formation of AgNPs on the surfaces of AgNWs was confirmed by multiple characterization methods including scanning electron microscopy(SEM),transmission electron microscope(TEM),atomic force microscopy(AFM) and X-ray diffraction(XRD).The results show that the fluorescence intensity of the poly(3-hexylthiophene)(P3HT) on the composite structure was greatly enhanced compared with that on bare glass substrate,and the intensity increased with the increase in particle sizes and density.The mechanism was basedo n the increase in excitation rate and the radiation decay rate.The new type of substrate could serve as a good and efficient MEF substrate for high-performance fluorescence-based devices.展开更多
The spectral properties of trivalent erbium ions(Er^3+) are systematically studied in a melt-quenched germanate glass(60 GeO2-20PbO-10BaO-10K2O-0.1Ag2O) containing silver(Ag) particles.Thermal treatment of the ...The spectral properties of trivalent erbium ions(Er^3+) are systematically studied in a melt-quenched germanate glass(60 GeO2-20PbO-10BaO-10K2O-0.1Ag2O) containing silver(Ag) particles.Thermal treatment of the material leads to the precipitation of Ag particles as observed by transmission electron microscopy and confirmed by absorption spectrum for the obvious surface plasmon resonance peak of Ag particles.The fluorescence from Er^3+ in the 10-min-annealed sample with Ag particles is found to be 4.2 times enhanced compared with the unannealed sample excited by 488-nm Ar+ laser.A comparison is made between a spectral study performed on the unannealed Er^3+-doped sample and the one annealed for 20 min.The data of absorption cross section and Judd-Ofelt intensity parameters show the agreement between the two samples no matter whether there are Ag particles,indicating that the introduction of Ag particles by post-heat treatment has no effect on the crystal field environment of Er^3+ ions.The fluorescence enhancement is attributed to the surface plasmon oscillations of Ag particles in germanate glass.展开更多
A novel β-diketone, 1-(3,4,5-trisbenzyloxy)benzoyl-5-benzoyl acetylacetone (TBAA), and its corresponding binary Tb(Ⅲ) complex Tb(TBAA)3·2H2O and ternary complex Tb(TBAA)3Phen with 1,10-phenanthroline ...A novel β-diketone, 1-(3,4,5-trisbenzyloxy)benzoyl-5-benzoyl acetylacetone (TBAA), and its corresponding binary Tb(Ⅲ) complex Tb(TBAA)3·2H2O and ternary complex Tb(TBAA)3Phen with 1,10-phenanthroline (Phen) were prepared. The ligand was characterized based on elemental analysis, FT-IR, and 1H NMR. The complexes were characterized with elemental analysis, FT-IR and thermogravimetry and derivative thermogravimetry (TG-DTG). Photoluminescence measurements indicated that the energy absorbed by the organic ligand was efficiently transferred to the central Tb3+ ions, and the complex showed intense and characteristic emissions due to the 5D4→7FJ transitions of the central Tb3+ ions. Both complexes showed longer fluorescence lifetimes. After the introduction of the second ligand Phen group, the relative emission intensities and fluorescence lifetimes of the ternary complex Tb(TBAA)3Phen enhanced more obviously than that of the binary complex Tb(TBAA)3·2H2O. This indicated that the presence of the ligand TBAA and the second ligand Phen could sensitize fluorescence intensities of Tb(Ⅲ) ions, and the introduction of Phen group resulted in the enhancement of the fluorescence properties of the Tb(Ⅲ) ternary rare earth complex.展开更多
Fluorescence and cofluorescence properties of Tb(Ⅲ) solid complexes werestudied using pyromellitic acid (PMA) as ligand and fluorescence inert ions as doping elements. Thecofluorescence enhancement, a result of ligan...Fluorescence and cofluorescence properties of Tb(Ⅲ) solid complexes werestudied using pyromellitic acid (PMA) as ligand and fluorescence inert ions as doping elements. Thecofluorescence enhancement, a result of ligand sensitized fluorescence, was observed in Tb(Ⅲ) solidcomplexes doped with fluorescent inert ions La(Ⅲ), Gd(Ⅲ), Ca(Ⅲ), and Sr(Ⅲ). The effect of thetype and content of doping elements on fluorescence enhancement was studied, and optimum conditionswere determined. The results show that Gd (La, Ca, Sr) has clear cofluorescence effect in solidcomplex Tb-M-PMA system, and in present work, rare earth complex fluorescent powder that emitsbright green fluorescence at ultraviolet excitation was obtained, which had potential application asfluorescent anti-counterfeit ink.展开更多
We fabricate nano-structural metal films to improve photoluminescence of perovskite films. When the perovskite film is placed on an ammonia-treated alumina film, stronger photoluminescence is found due to local field ...We fabricate nano-structural metal films to improve photoluminescence of perovskite films. When the perovskite film is placed on an ammonia-treated alumina film, stronger photoluminescence is found due to local field en- hancement effects. In addition, the oxide spacer layer between the metal (e.g., AI, Ag and Au) substrate and the perovskite film plays an important role. The simulations and experiments imply that the enhancement is related to surface plasmons of nano-structural metals.展开更多
The effect of cucurbit[7]uril(CB[7]) on fluorescence properties and biocompatibility of the bis-viologen biphenyl molecule(BPV22+) was investigated by using 1 H NMR spectroscopy,fluorescence emission titration,and in ...The effect of cucurbit[7]uril(CB[7]) on fluorescence properties and biocompatibility of the bis-viologen biphenyl molecule(BPV22+) was investigated by using 1 H NMR spectroscopy,fluorescence emission titration,and in vitro cytotoxicity experiments.CB[7] can be combined with BPV22+ in a stoichiometric ratio of 1:1 and 2:1.After the formation of host-vip complex,the fluorescence emission intensity of BPV22+ increased significantly,and the emission spectrum blue shifted.Meanwhile,the host-vip complexes showed better biocompatibility than BPV22+ in cell cytotoxicity studies.Results of this paper lay a foundation for the development of host-vip type of fluo rescent probes,biological imaging and so forth.展开更多
Enhancement of uorescent radiation is of great importance for applications including biological imaging,high-sensitivity detectors,and integrated light sources.Strong electromagnetic elds can be created around metalli...Enhancement of uorescent radiation is of great importance for applications including biological imaging,high-sensitivity detectors,and integrated light sources.Strong electromagnetic elds can be created around metallic nanoparticles or in gap of nanostructures,where the local state density of radiating mode is then dramatically enhanced.While enhanced uorescent emission has been demonstrated in many metallic nanoparticles and nanoparticle pairs,simultaneous mediation of absorption and emission processes of uorescent emitters remains challenging in metallic nanostructures.Here,we investigate uorescent emission mediated by metal-dielectric-metal fishnet metasurface,in which localized surface plasmon(LSP)and magnetic plasmon polaritons(MPPs)modes are coupled with absorption and emission processes,respectively.For absorption process,coupling of the LSP mode enables spatially-selective excitation of the uorescent emitters by rotating the polarization of the pump laser beam.In addition,the polarization-dependent MPP mode enables manipulation of both polarization and wavelength of the uorescent emission by introducing a rectangular fishnet structure.All the experimental observations are further corroborated by nite-difference time-domain simulations.The structure reported here has great potential for application to color light-emitting devices and nanoscale integrated light sources.展开更多
文摘Bay-site carboxyl functionalized perylene diimide derivative 1,7-COOH-PDI-C_(12)(PDI-COOH)was synthesized and distinct enhanced fluorescence was observed through combining with calcium ion(Ca^(2+))in THF/H_(2)O solution.The assembly and fluorescence behavior of PDI-COOH/Ca^(2+)were studied in detail by changing hydration state with different concentrations.Based on the differences in assembly morphology and stoichiometric ratios of PDICOOH/Ca^(2+),we proposed the fluorescence emission mechanism of PDI-COOH/Ca^(2+)in THF/H_(2)O and THF,respectively.This work reveals a novel strategy of aggregated state fluorescence enhancement and reminds us of the important role of water in molecular fluorescence emission and assembly.
基金Supported by the National Natural Science Foundation of China(21775114,21874102)。
文摘Silver ion(Ag^(+))is a highly toxic metal ion,and its monitoring in water or food resources has become extraordinarily necessary within the scope of human health.In the light of the fact of Ag^(+)-induced folding structure of specific peptides,an unlabeled and highselectivity Ag^(+)assay is presented by means of intrinsic fluorescence of peptides.Under the quenching effect of gold nanoparticles(AuNPs),characteristic fluorescence of peptides could be considerably reduced by rapid modification.Along with the Ag adding,the fluorescence signals of peptide-AuNPs are largely enhanced by the behavior between peptides and Agt.This is basically involving the formation of 4-coordinated complexes,generating the changes of peptides in structure and fluorescence properties.Under this circumstance,the adverse influence of plenty of interfering ions is suppressed,including the toxic Hg^(2+),Pb^(2+).The results highlight that Ag ions could be selectively recognized as low as 2.4 nmol/L with a linear range of 5 to 800 nmol/L.In comparison with other programs,the given approach declares simplicity,sensitivity,and superior selectivity.Furthermore,the biosensor excels in the practical application in water samples(e.g.,lake,tap and drinking water)owing to its non-interference and on-site rapid determination.
基金supported by the National Natural Science Foundation of China(Nos.22175129,22475149)the International Sci-Tech Cooperation Project under the“Innovation Yongjiang 2035”Key R&D Programme of Ningbo Municipality(No.2024H017).
文摘Perylene diimide(PDI)derivatives have emerged as a class of important organic fluorescent materials owing to their high extinction coefficient,excellent thermal and photostability,and versatile structural tunability.However,due to its intrinsic rigid planar structure,π-πstacking is easy to occur,resulting in aggregation-caused quenching(ACQ).In recent years,extensive efforts have been devoted to overcome this challenge and enhance the fluorescence performance of PDIs.This review systematically summarizes representative strategies from three major perspectives:(i)Rational molecular design,including the introduction of bulky aromatic substituents,dendritic or polyhedral oligomeric silsesquioxane(POSS)units to provide steric hindrance,as well as the activation of aggregation-induced emission(AIE);(ii)Polymer-based regulation strategies,including physical blending with polymer hosts and covalent integration into polymer backbones,which provide spatial isolation and structural robustness;and(iii)Supramolecular assembly,where host-vip inclusion and self-assembly pathways precisely tune intermolecular packing and excitonic coupling.These strategies have enabled significant improvements in fluorescence quantum yield(FLQY)across solution,aggregate,and solid states.Furthermore,highly emissive perylene diimide(PDI)derivatives have demonstrated broad applicability in biomedicine,sensing and anti-counterfeiting,and optoelectronic devices such as organic light-emitting diodes(OLEDs).This review highlights the fundamental design principles,performance optimization strategies,and emerging application frontiers of PDI-based luminescent materials,providing guidance for their further development toward multifunctional and sustainable optoelectronic technologies.
基金the National Natural Science Foundation of China(22078051,22478063,22408035)the Fundamental Research Funds for the Central Universities(DUT22-LAB610)the Open Fund of the Key Laboratory of Advanced Display and System Applications,Ministry of Education,Shanghai University(OF202401)for financial support of this work.
文摘Most of acridine based thermally activated delayed fluorescence(TADF)emitters are characterized by advantageous reverse intersystem crossing(RISC)rate(kRISCs)due to the perpendicular orientation of the acridine donor to the acceptor moiety,but suffer from a poor radiation rate(kr)typically in the order of 10^(6) s^(−1).Herein,two sky blue TADF emitters 3,6-DMAC-AD-Py and 3,6-SFAC-AD-Py were developed by linking acridine(DMAC)and spiro-fluorene-acridine(SFAC)donors to 10-(pyridin-2-yl)acridin-9(10H)-one(AD-Py)acceptor.Larger SFAC and electron-deficient pyridyl groups are deliberately incorporated in 3,6-SFACAD-Py since the unique through-space interaction between them is designed to drive the rotation of inner acridine ring in SFAC for enhancing frontier molecular orbitals overlap while keeping a decent TADF behavior.Thus,the kr of 3,6-SFACAD-Py is increased to 1.5×10^(7) s^(−1).Simultaneously,SFAC donors improve spin orbital coupling strength and reduce the energy gaps,generating kRISC of 1.8×10^(6) s^(−1).This is the first acridine donor based TADF emitter realizing kr of 10^(7) s^(−1) and kRISC of 10^(6) s^(−1) by a through-space interaction strategy.3,6-SFACAD-Py enables a highly efficient sky-blue organic light-emitting diode with a maximum external quantum efficiency(EQE)of 34.7%and Commission International de I'Eclairage coordinates of(0.19,0.37).More importantly,the EQE still remained 27.6%and 16.9%at high brightness of 1000 and 10,000 cd m^(−2).
文摘Over the past ten years,numerous papers have been published on the use of indocyanine green(ICG)fluorescence in liver surgery for hepatocellular carcinoma(HCC).There are many different applications.The first involves targeting superficial tumors in patients with macronodular cirrhosis and an irregular liver surface.In a minimally invasive setting,the lack of tactile feedback on the hepatic surface makes detecting subcapsular HCC with ultrasound alone challenging.ICG fusion images can mimic the tactile feedback of the hand and act as an ultrasound booster.ICG fluorescence can be used to evaluate tumor residues after minimally invasive thermal ablation.ICG fluorescence imaging can also be used to identify the grade of HCC early on and evaluate the microinvasive component.
基金funded by the National Natural Science Foundation of China,grant numbers 52374156 and 62476005。
文摘Images taken in dim environments frequently exhibit issues like insufficient brightness,noise,color shifts,and loss of detail.These problems pose significant challenges to dark image enhancement tasks.Current approaches,while effective in global illumination modeling,often struggle to simultaneously suppress noise and preserve structural details,especially under heterogeneous lighting.Furthermore,misalignment between luminance and color channels introduces additional challenges to accurate enhancement.In response to the aforementioned difficulties,we introduce a single-stage framework,M2ATNet,using the multi-scale multi-attention and Transformer architecture.First,to address the problems of texture blurring and residual noise,we design a multi-scale multi-attention denoising module(MMAD),which is applied separately to the luminance and color channels to enhance the structural and texture modeling capabilities.Secondly,to solve the non-alignment problem of the luminance and color channels,we introduce the multi-channel feature fusion Transformer(CFFT)module,which effectively recovers the dark details and corrects the color shifts through cross-channel alignment and deep feature interaction.To guide the model to learn more stably and efficiently,we also fuse multiple types of loss functions to form a hybrid loss term.We extensively evaluate the proposed method on various standard datasets,including LOL-v1,LOL-v2,DICM,LIME,and NPE.Evaluation in terms of numerical metrics and visual quality demonstrate that M2ATNet consistently outperforms existing advanced approaches.Ablation studies further confirm the critical roles played by the MMAD and CFFT modules to detail preservation and visual fidelity under challenging illumination-deficient environments.
基金financially sponsored by the National Natural Science Foundation of China(No.52204414)the National Energy-Saving and Low-Carbon Materials Production and Application Demonstration Platform Program,China(No.TC220H06N)+1 种基金the National Key R&D Program of China(No.2021YFC1910504)the Fundamental Research Funds for the Central Universities,China(No.FRFTP-20-097A1Z)。
文摘MnO_(x)-CeO_(2)catalysts for the low-temperature selective catalytic reduction(SCR)of NO remain vulnerable to water and sulfur poisoning,limting their practical applications.Herein,we report a hydrophobic-modified MnO_(x)-CeO_(2)catalyst that achieves enhanced NO conversion rate and stability under harsh conditions.The catalyst was synthesized by decorating MnOx crystals with amorphous CeO_(2),followed by loading hydrophobic silica on the external surfaces.The hydrophobic silica allowed the adsorption of NH_(3)and NO and diffusion of H,suppressed the adsorption of H_(2)O,and prevented SO_(2)interaction with the Mn active sites,achieving selective molecular discrimination at the catalyst surface.At 120℃,under H_(2)O and SO_(2)exposure,the optimal hydrophobic catalyst maintains 82%NO conversion rate compared with 69%for the unmodified catalyst.The average adsorption energies of NH_(3),H_(2)O,and SO_(2)decreased by 0.05,0.43,and 0.52 eV,respectively.The NO reduction pathway follows the Eley-Rideal mechanism,NH_(3)^(*)+*→NH_(2)^(*)+H^(*)followed by NH_(2)^(*)+NO^(*)→N_(2)^(*)+H_(2)O^(*),with NH_(3)dehydrogenation being the rate determining step.Hydrophobic modification increased the activation energy for H atom transfer,leading to a minor decrease in the NO conversion rate at 120℃.This work demonstrates a viable strategy for developing robust NH_(3)-S CR catalysts capable of efficient operation in water-and sulfur-rich environments.
基金supported by the National Natural Science Foundation of China(Nos.92461304 and 52202192)China Postdoctoral Science Foundation(Nos.2020M682338 and 2023T160593)+2 种基金China National Postdoctoral Program for Innovative Talents(No.BX20230329)Zhengzhou Universitythe support from the Center of New Materials and Device of Huazhong University of Science and Technology.
文摘Two-dimensional(2D)MoS_(2) is considered an excellent candidate material for nextgeneration photodetectors.However,the high dark current and low photocurrent in MoS_(2) devices severely hinder their practical application.Strategies for suppressing dark current and enhancing photocurrent should be explored.Herein,we propose a modification strategy for MoS_(2) by utilizing Ag_(70) nanoclusters(NCs)as electron reservoirs and photoabsorbers to suppress dark current and enhance the photocurrent of 2D MoS_(2) photodetector.Remarkably,the dark current is effectively suppressed by four orders of magnitude,while the photocurrent is enhanced by over tenfold upon modification with Ag_(70) NCs,compared to the pristine MoS_(2) photodetector.The reduction in dark current is attributed to charge transfer from MoS_(2) to Ag_(70) NCs owing to the strong electronwithdrawing property of Ag_(70) NCs.The increase in photocurrent benefits from enhanced optical absorption of the photodetector after Ag_(70) NCs modification and the subsequent injection of photoexcited electrons from Ag_(70) NCs to MoS_(2).Compared to isolated MoS_(2),the modulated photodetector shows exceptional improvements in several key figures of merit(such as responsivity,detectivity,external quantum efficiency,and photoswitching on/off ratio).This study opens up new avenues for building high-performance 2D MoS_(2) photodetectors.
基金supported by the Zhongyuan University of Technology Discipline Backbone Teacher Support Program Project(No.GG202417)the Key Research and Development Program of Henan under Grant 251111212000.
文摘Lateral movement represents the most covert and critical phase of Advanced Persistent Threats(APTs),and its detection still faces two primary challenges:sample scarcity and“cold start”of new entities.To address these challenges,we propose an Uncertainty-Driven Graph Embedding-Enhanced Lateral Movement Detection framework(UGEA-LMD).First,the framework employs event-level incremental encoding on a continuous-time graph to capture fine-grained behavioral evolution,enabling newly appearing nodes to retain temporal contextual awareness even in the absence of historical interactions and thereby fundamentally mitigating the cold-start problem.Second,in the embedding space,we model the dependency structure among feature dimensions using a Gaussian copula to quantify the uncertainty distribution,and generate augmented samples with consistent structural and semantic properties through adaptive sampling,thus expanding the representation space of sparse samples and enhancing the model’s generalization under sparse sample conditions.Unlike static graph methods that cannot model temporal dependencies or data augmentation techniques that depend on predefined structures,UGEA-LMD offers both superior temporaldynamic modeling and structural generalization.Experimental results on the large-scale LANL log dataset demonstrate that,under the transductive setting,UGEA-LMD achieves an AUC of 0.9254;even when 10%of nodes or edges are withheld during training,UGEA-LMD significantly outperforms baseline methods on metrics such as recall and AUC,confirming its robustness and generalization capability in sparse-sample and cold-start scenarios.
基金V. ACKNOWLEDGMENTS This work was supported by the National Natural Science Foundation of China (No.21071136), the National Basic Research Program of China (No.2010CB934700and No.2012CB932001), the Research FUnd for the Doctoral Program of Higher Education of China (No.20103402110033) and Anhui Provincial Education Department (No.KJ2012ZD11).
文摘Monodisperse Ag nanoparticles with diameters of about 3.4 nm were synthesized by a facile ultrasonic synthetic route at room temperature with the reduction of borane-tert-butylamine in the presence of oleylamine (OAm) and oleic acid (OA). The reaction parameters of time, the molar ratios of OAm to OA were studied, and it was found that these parameters played important roles in the morphology and size of the products. Meanwhile, surface enhanced Raman spectrum (SERS) property suggested the Ag nanoparticles exhibited high SERS effect on the model molecule Rhodamine 6G. And also, two-photon fluorescence images showed that the silver nanoparticles had high performances in fluorescence enhancement.
基金supported by the National Natural Science Foundation of China(No.20332020,No.20472079).
文摘A series of fluorescent chemosensors 1-3 were synthesized to detect transition metal ions. At the room temperature, fluorescence intensities of these chemosensors in acetonitrile without transition metal ions were found to be very weak, due to the process of the efficient intramolecular photoinduced electron transfer (PET). However, after addition of the transition metal ions, the chemoscnsor 1-3 exhibits obvious fluorescence enhancement. Moreover, the intensity of the fluorescence emission of chemosensors increases significantly in the presence of Zn^2+ and Cd^2+. The fluorescent chemosensors with different polyamine as receptors show diverse affinity abilities to the transition metal ions and signal the receptor-metal ion interaction by the intensity change of fluorescence emission.
基金Financial supports from the National Natural Science Foundation of China(No.51073144)Natural Science Foundation of Anhui Education Department(No.KJ2011B051)
文摘A novel fluorescent aqueous polyurethane emulsion DDAQ-TDI-PU was synthesized by blocking the anthraquinone moiety of 1,4-diamino-2,3-diphenoxyanthraquinone(DDAQ) into polyurethane chain using 2,4-tolylene diisocyanate(TDI),poly(propylene glycol) and 2,2-dimethylol propionic acid.The chain structure of DDAQ-TDI-PU was confirmed by means of Fourier transform infrared spectroscopy and UV-vis analysis.Comparing to the UV-vis spectrum of DDAQ,DDAQ-TDI-PU showed a hypsochromic shift from the absorption maxima of 518,558,609 nm to 510,548,586 nm,respectively.It was found that the fluorescence intensity of DDAQ-TDI-PU emulsion was enhanced greatly comparing with that of DDAQ.The fluorescence of DDAQ-TDI-PU was very stable not only for the long term storage but also for the fluorescence quencher.
基金This work was financially supported by the Science Foundation of Hunan Province, China (No. 01C030)
文摘The fluorescence of terbium (Ⅲ) was enhanced by about three orders of magnitude in the presence of trimellitic acid (benzene-1, 2, 4-tricarboxylic acid (TLA)) in aqueous solution at pH 6. The fluorescence intensity could be greatly increased when the system of Tb^3+-TLA was treated with La^3+ (or Gd^3+) and TritonX- 100. The addition of La^3+ (or Gd^3+) enhanees the fluorescence of the system by about two orders of magnitude due to cofluorescenee, and the TritonX-100 micellar medium plays an important role for stabilization of the system. Both the intermolecular energy transfer mode and intramolecular energy transfer mode are responsible for the mechanism of fluorescence enhancement. In the optimum condi- tions, the fluorescence intensity is a linear function of Tb3~ concentration in the range of 7.8 × 10^-9-3.6 × 10^4 mol/L for the system Tb^3+-La^3+-TLA and 1.0 × 10^-8-4.7 × 10^-5 mol/L for the system Tb^3+-Gd^3+-TLA, and the limits of detection are 4.6 × 10^-10 mol/L and 6.0 × 10^-10 mol/L, respectively.
基金financially supported by the National Natural Science Foundation of China (No.51273048)Science and Technology Planning Project of Guangdong Province (No.2017B090915004)the Open Operation of Guangdong Provincial Key Laboratory of Advanced Coatings Research and Development (No.2017B030314105)
文摘A new substrate,aligned Ag nanowires decorated with silver nanoparticle composite structure(AgNWs@AgNPs),was fabricated to investigate metalenhanced fluorescence(MEF) and its mechanism.The new composite structure was fabricated via a three-phase interface assembly method followed by SnCl2 sensitization and AgNO3 reduction process.The size and distribution of the nanoparticles on silver nanowires increased with the sensitization and reduction cycles.The formation of AgNPs on the surfaces of AgNWs was confirmed by multiple characterization methods including scanning electron microscopy(SEM),transmission electron microscope(TEM),atomic force microscopy(AFM) and X-ray diffraction(XRD).The results show that the fluorescence intensity of the poly(3-hexylthiophene)(P3HT) on the composite structure was greatly enhanced compared with that on bare glass substrate,and the intensity increased with the increase in particle sizes and density.The mechanism was basedo n the increase in excitation rate and the radiation decay rate.The new type of substrate could serve as a good and efficient MEF substrate for high-performance fluorescence-based devices.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 61078061 and 11104023)the Natural Science Foundation of Liaoning Province,China (Grant No. 20111032)+1 种基金the State Key Development Program for Basic Research of China (Grant No. 2012CB626801)the Fundamental Research Funds for the Central Universities (Grant No. 2011QN152)
文摘The spectral properties of trivalent erbium ions(Er^3+) are systematically studied in a melt-quenched germanate glass(60 GeO2-20PbO-10BaO-10K2O-0.1Ag2O) containing silver(Ag) particles.Thermal treatment of the material leads to the precipitation of Ag particles as observed by transmission electron microscopy and confirmed by absorption spectrum for the obvious surface plasmon resonance peak of Ag particles.The fluorescence from Er^3+ in the 10-min-annealed sample with Ag particles is found to be 4.2 times enhanced compared with the unannealed sample excited by 488-nm Ar+ laser.A comparison is made between a spectral study performed on the unannealed Er^3+-doped sample and the one annealed for 20 min.The data of absorption cross section and Judd-Ofelt intensity parameters show the agreement between the two samples no matter whether there are Ag particles,indicating that the introduction of Ag particles by post-heat treatment has no effect on the crystal field environment of Er^3+ ions.The fluorescence enhancement is attributed to the surface plasmon oscillations of Ag particles in germanate glass.
基金Project supported by Shanxi (20072194 and 20072185) Provincial Youth Technology Research Foundationthe Foundation of Taiyuan Graduate Innovation (100115133 and 100115131)
文摘A novel β-diketone, 1-(3,4,5-trisbenzyloxy)benzoyl-5-benzoyl acetylacetone (TBAA), and its corresponding binary Tb(Ⅲ) complex Tb(TBAA)3·2H2O and ternary complex Tb(TBAA)3Phen with 1,10-phenanthroline (Phen) were prepared. The ligand was characterized based on elemental analysis, FT-IR, and 1H NMR. The complexes were characterized with elemental analysis, FT-IR and thermogravimetry and derivative thermogravimetry (TG-DTG). Photoluminescence measurements indicated that the energy absorbed by the organic ligand was efficiently transferred to the central Tb3+ ions, and the complex showed intense and characteristic emissions due to the 5D4→7FJ transitions of the central Tb3+ ions. Both complexes showed longer fluorescence lifetimes. After the introduction of the second ligand Phen group, the relative emission intensities and fluorescence lifetimes of the ternary complex Tb(TBAA)3Phen enhanced more obviously than that of the binary complex Tb(TBAA)3·2H2O. This indicated that the presence of the ligand TBAA and the second ligand Phen could sensitize fluorescence intensities of Tb(Ⅲ) ions, and the introduction of Phen group resulted in the enhancement of the fluorescence properties of the Tb(Ⅲ) ternary rare earth complex.
基金This work is financially supported by the Natural Science Foundation of Hunan Province (No. 01JJY3004) and Technology of China National Packaging Corporation.
文摘Fluorescence and cofluorescence properties of Tb(Ⅲ) solid complexes werestudied using pyromellitic acid (PMA) as ligand and fluorescence inert ions as doping elements. Thecofluorescence enhancement, a result of ligand sensitized fluorescence, was observed in Tb(Ⅲ) solidcomplexes doped with fluorescent inert ions La(Ⅲ), Gd(Ⅲ), Ca(Ⅲ), and Sr(Ⅲ). The effect of thetype and content of doping elements on fluorescence enhancement was studied, and optimum conditionswere determined. The results show that Gd (La, Ca, Sr) has clear cofluorescence effect in solidcomplex Tb-M-PMA system, and in present work, rare earth complex fluorescent powder that emitsbright green fluorescence at ultraviolet excitation was obtained, which had potential application asfluorescent anti-counterfeit ink.
基金Supported by the Ministry of Science and Technology of China under Grant No 2016YFA0202201the National Natural Science Foundation of China under Grant Nos 61290304,11574335 and 61376016+1 种基金the Youth Innovation Promotion Association of the Chinese Academy of Sciencesthe 333 Project of Jiangsu province under Grant No BRA2017352
文摘We fabricate nano-structural metal films to improve photoluminescence of perovskite films. When the perovskite film is placed on an ammonia-treated alumina film, stronger photoluminescence is found due to local field en- hancement effects. In addition, the oxide spacer layer between the metal (e.g., AI, Ag and Au) substrate and the perovskite film plays an important role. The simulations and experiments imply that the enhancement is related to surface plasmons of nano-structural metals.
基金supported by the National Natural Science Foundation of China (No.21374055)the Fundamental Research Funds of Shandong University (No.11190078614092)。
文摘The effect of cucurbit[7]uril(CB[7]) on fluorescence properties and biocompatibility of the bis-viologen biphenyl molecule(BPV22+) was investigated by using 1 H NMR spectroscopy,fluorescence emission titration,and in vitro cytotoxicity experiments.CB[7] can be combined with BPV22+ in a stoichiometric ratio of 1:1 and 2:1.After the formation of host-vip complex,the fluorescence emission intensity of BPV22+ increased significantly,and the emission spectrum blue shifted.Meanwhile,the host-vip complexes showed better biocompatibility than BPV22+ in cell cytotoxicity studies.Results of this paper lay a foundation for the development of host-vip type of fluo rescent probes,biological imaging and so forth.
基金supported by the National Nature Science Foundation of China(No.11674303 and No.11574293)the USTC Center for Micro and Nanoscale Research and Fabrication
文摘Enhancement of uorescent radiation is of great importance for applications including biological imaging,high-sensitivity detectors,and integrated light sources.Strong electromagnetic elds can be created around metallic nanoparticles or in gap of nanostructures,where the local state density of radiating mode is then dramatically enhanced.While enhanced uorescent emission has been demonstrated in many metallic nanoparticles and nanoparticle pairs,simultaneous mediation of absorption and emission processes of uorescent emitters remains challenging in metallic nanostructures.Here,we investigate uorescent emission mediated by metal-dielectric-metal fishnet metasurface,in which localized surface plasmon(LSP)and magnetic plasmon polaritons(MPPs)modes are coupled with absorption and emission processes,respectively.For absorption process,coupling of the LSP mode enables spatially-selective excitation of the uorescent emitters by rotating the polarization of the pump laser beam.In addition,the polarization-dependent MPP mode enables manipulation of both polarization and wavelength of the uorescent emission by introducing a rectangular fishnet structure.All the experimental observations are further corroborated by nite-difference time-domain simulations.The structure reported here has great potential for application to color light-emitting devices and nanoscale integrated light sources.