In order to analyze the heterogeneity in vehicular traffic speed, a new method that integrates cluster analysis and probability distribution function fitting is presented. First, for identifying the optimal number of ...In order to analyze the heterogeneity in vehicular traffic speed, a new method that integrates cluster analysis and probability distribution function fitting is presented. First, for identifying the optimal number of clusters, the two-step cluster method is applied to analyze actual speed data, which suggests that dividing speed data into two clusters can best reflect the intrinsic patterns of traffic flows. Such information is then taken as guidance in probability distribution function fitting. The normal, skew-normal and skew-t distribution functions are used to fit the probability distribution of each cluster respectively, which suggests that the skew-t distribution has the highest fitting accuracy; the second is skew-normal distribution; the worst is normal distribution. Model analysis results demonstrate that the proposed mixture model has a better fitting and generalization capability than the conventional single model. In addition, the new method is more flexible in terms of data fitting and can provide a more accurate model of speed distribution.展开更多
Under hydrothermal and solvothermal conditions,two novel cobalt-based complexes,{[Co_(2)(CIA)(OH)(1,4-dtb)]·3.2H_(2)O}n(HU23)and{[Co_(2)(CIA)(OH)(1,4-dib)]·3.5H2O·DMF}n(HU24),were successfully construct...Under hydrothermal and solvothermal conditions,two novel cobalt-based complexes,{[Co_(2)(CIA)(OH)(1,4-dtb)]·3.2H_(2)O}n(HU23)and{[Co_(2)(CIA)(OH)(1,4-dib)]·3.5H2O·DMF}n(HU24),were successfully constructed by coordinatively assembling the semi-rigid multidentate ligand 5-(1-carboxyethoxy)isophthalic acid(H₃CIA)with the Nheterocyclic ligands 1,4-di(4H-1,2,4-triazol-4-yl)benzene(1,4-dtb)and 1,4-di(1H-imidazol-1-yl)benzene(1,4-dib),respectively,around Co^(2+)ions.Single-crystal X-ray diffraction analysis revealed that in both complexes HU23 and HU24,the CIA^(3-)anions adopt aκ^(7)-coordination mode,bridging six Co^(2+)ions via their five carboxylate oxygen atoms and one ether oxygen atom.This linkage forms tetranuclear[Co4(μ3-OH)2]^(6+)units.These Co-oxo cluster units were interconnected by CIA^(3-)anions to assemble into 2D kgd-type structures featuring a 3,6-connected topology.The 2D layers were further connected by 1,4-dtb and 1,4-dib,resulting in 3D pillar-layered frameworks for HU23 and HU24.Notably,despite the similar configurations of 1,4-dtb and 1,4-dib,differences in their coordination spatial orientations lead to topological divergence in the 3D frameworks of HU23 and HU24.Topological analysis indicates that the frameworks of HU23 and HU24 can be simplified into a 3,10-connected net(point symbol:(4^(10).6^(3).8^(2))(4^(3))_(2))and a 3,8-connected tfz-d net(point symbol:(4^(3))_(2)((4^(6).6^(18).8^(4)))),respectively.This structural differentiation confirms the precise regulatory role of ligands on the topology of metal-organic frameworks.Moreover,the ultraviolet-visible absorption spectra confirmed that HU23 and HU24 have strong absorption capabilities for ultraviolet and visible light.According to the Kubelka-Munk method,their bandwidths were 2.15 and 2.08 eV,respectively,which are consistent with those of typical semiconductor materials.Variable-temperature magnetic susceptibility measurements(2-300 K)revealed significant antiferromagnetic coupling in both complexes,with their effective magnetic moments decreasing markedly as the temperature lowered.CCDC:2457554,HU23;2457553,HU24.展开更多
Effective control of gas-phase pollutants(volatile organic compounds(VOCs)and CO)is critical to human health and the ecological environment.Catalytic oxidation is one of the most promising technologies for achieving e...Effective control of gas-phase pollutants(volatile organic compounds(VOCs)and CO)is critical to human health and the ecological environment.Catalytic oxidation is one of the most promising technologies for achieving efficient volatile organic compounds and CO emission control.The subnano cluster catalyst can not only provide catalytic sites with multiple metal atoms,but also maintain full utilization efficiency.Almost all metal atoms in highly dispersed clusters can be used for adsorption and conversion of reactants.Recently,various types of sub-nano clusters,including subnano cluster oxides,have been developed and demonstrated excellent performance in low-temperature gas-phase pollutants combustion.In this mini review,we systematically summarize the structure,physicochemical properties,characterization,and applications of sub-nano cluster catalysts in catalytic oxidation of CO,methane,propane,propylene,toluene and its derivatives,formaldehyde and chlorinated volatile organic compounds.Finally,we have analyzed and discussed the problems and challenges faced by sub-nano cluster catalysts in both basic research and practical applications,providing a scientific basis for the design,synthesis,and application of efficient heterogeneous catalysts for CO and VOCs oxidation.展开更多
This paper proposes an equivalent modeling method for photovoltaic(PV)power stations via a particle swarm optimization(PSO)K-means clustering(KMC)algorithm with passive filter parameter clustering to address the compl...This paper proposes an equivalent modeling method for photovoltaic(PV)power stations via a particle swarm optimization(PSO)K-means clustering(KMC)algorithm with passive filter parameter clustering to address the complexities,simulation time cost and convergence problems of detailed PV power station models.First,the amplitude–frequency curves of different filter parameters are analyzed.Based on the results,a grouping parameter set for characterizing the external filter characteristics is established.These parameters are further defined as clustering parameters.A single PV inverter model is then established as a prerequisite foundation.The proposed equivalent method combines the global search capability of PSO with the rapid convergence of KMC,effectively overcoming the tendency of KMC to become trapped in local optima.This approach enhances both clustering accuracy and numerical stability when determining equivalence for PV inverter units.Using the proposed clustering method,both a detailed PV power station model and an equivalent model are developed and compared.Simulation and hardwarein-loop(HIL)results based on the equivalent model verify that the equivalent method accurately represents the dynamic characteristics of PVpower stations and adapts well to different operating conditions.The proposed equivalent modeling method provides an effective analysis tool for future renewable energy integration research.展开更多
Although k-nearest neighbors （KNN） is a popular fingerprint match algorithm for its simplicity and accuracy, because it is sensitive to the circumstances, a fuzzy c-means （FCM） clustering algorithm is applied to i...Although k-nearest neighbors （KNN） is a popular fingerprint match algorithm for its simplicity and accuracy, because it is sensitive to the circumstances, a fuzzy c-means （FCM） clustering algorithm is applied to improve it. Thus, a KNN-based two-step FCM weighted （KTFW） algorithm for indoor positioning in wireless local area networks （WLAN） is presented in this paper. In KTFW algorithm, k reference points （RPs） chosen by KNN are clustered through FCM based on received signal strength （RSS） and location coordinates. The right clusters are chosen according to rules, so three sets of RPs are formed including the set of k RPs chosen by KNN and are given different weights. RPs supposed to have better contribution to positioning accuracy are given larger weights to improve the positioning accuracy. Simulation results indicate that KTFW generally outperforms KNN and its complexity is greatly reduced through providing initial clustering centers for FCM.展开更多
Nanoclusters consisting of a few atoms have attracted a lot of research interests due to their exotic size-dependent properties. Here, well-ordered two-dimensional Sb cluster superlattice was fabricated on Si substrat...Nanoclusters consisting of a few atoms have attracted a lot of research interests due to their exotic size-dependent properties. Here, well-ordered two-dimensional Sb cluster superlattice was fabricated on Si substrate by a two-step method and characterized by scanning tunneling microscopy. High resolution scanning tunneling microscope measurements revealed the fine structures of the Sb clusters, which consist of several Sb atoms ranging from 2 to 7. Furthermore, the electronic structure of the nanocluster displays the quantized energy-level which is due to the single-electron tunneling effects. We believe that the fabrication of Sb cluster superlattice broadens the species of the cluster superlattice and provides a promising candidate to further explore the novel physical and chemical properties of the semimetal nanocluster.展开更多
Tin(Sn)-lead(Pb)mixed halide perovskites have attracted widespread interest due to their wider re-sponse wavelength and lower toxicity than lead halide perovskites,Among the preparation methods,the two-step method mor...Tin(Sn)-lead(Pb)mixed halide perovskites have attracted widespread interest due to their wider re-sponse wavelength and lower toxicity than lead halide perovskites,Among the preparation methods,the two-step method more easily controls the crystallization rate and is suitable for preparing large-area per-ovskite devices.However,the residual low-conductivity iodide layer in the two-step method can affect carrier transport and device stability,and the different crystallization rates of Sn-and Pb-based per-ovskites may result in poor film quality.Therefore,Sn-Pb mixed perovskites are mainly prepared by a one-step method.Herein,a MAPb_(0.5)Sn_(0.5)I_(3)-based self-powered photodetector without a hole transport layer is fabricated by a two-step method.By adjusting the concentration of the ascorbic acid(AA)addi-tive,the final perovskite film exhibited a pure phase without residues,and the optimal device exhibited a high responsivity(0.276 A W^(-1)),large specific detectivity(2.38×10^(12) Jones),and enhanced stability.This enhancement is mainly attributed to the inhibition of Sn2+oxidation,the control of crystal growth,and the sufficient reaction between organic ammonium salts and bottom halides due to the AA-induced pore structure.展开更多
Based on DEA - Ridge Regression two-step method, the paper tries to construct industrial cluster competitiveness research framework for empirical analysis, and by the Hunan automobile industry cluster as an example. T...Based on DEA - Ridge Regression two-step method, the paper tries to construct industrial cluster competitiveness research framework for empirical analysis, and by the Hunan automobile industry cluster as an example. The study found that Hunan automobile industry cluster competitiveness is relatively weak, full of the very big promotion space; further research shows that the human capital investment, fixed capital investment, land investment and policy support are the main factors influencing the efficiency of automobile industry cluster in Hunan province.展开更多
A custom micro-arc oxidation(MAO)apparatus is employed to produce coatings under optimized constant voltage–current two-step power supply mode.Various analytical techniques,including scanning electron microscopy,conf...A custom micro-arc oxidation(MAO)apparatus is employed to produce coatings under optimized constant voltage–current two-step power supply mode.Various analytical techniques,including scanning electron microscopy,confocal laser microscopy,X-ray diffraction,X-ray photoelectron spectroscopy,transmission electron microscopy,and electrochemical analysis,are employed to characterize MAO coatings at different stages of preparation.MAO has MgO,hydroxyapatite,Ca_(3)(PO_(4))_(2),and Mg2SiO4 phases.Its microstructure of the coating is characterized by"multiple breakdowns,pores within pores",and"repaired blind pores".The porosity and the uniformity of MAO coating first declines in the constant voltage mode,then augments while the discharge phenomenon takes place,and finally decreases in the repair stage.These analyses reveal a four-stage growth pattern for MAO coatings:anodic oxidation stage,micro-arc oxidation stage,breakdown stage,and repairing stage.During anodic oxidation and MAO stages,inward growth prevails,while the breakdown stage sees outward and accelerated growth.Simultaneous inward and outward growth in the repair stage results in a denser,more uniform coating with increased thickness and improved corrosion resistance.展开更多
In existing studies, most slope stability analyses concentrate on conditions with constant temperature, assuming the slope is intact, and employ the Mohr-Coulomb (M-C) failure criterion for saturated soil to character...In existing studies, most slope stability analyses concentrate on conditions with constant temperature, assuming the slope is intact, and employ the Mohr-Coulomb (M-C) failure criterion for saturated soil to characterize the strength of the backfill. However, the actual working temperature of slopes varies, and natural phenomena such as rainfall and groundwater infiltration commonly result in unsaturated soil conditions, with cracks typically present in cohesive slopes. This study introduces a novel approach for assessing the stability of unsaturated soil stepped slopes under varying temperatures, incorporating the effects of open and vertical cracks. Utilizing the kinematic approach and gravity increase method, we developed a three-dimensional (3D) rotational wedge failure mechanism to simulate slope collapse, enhancing the traditional two-dimensional analyses. We integrated temperature-dependent functions and nonlinear shear strength equations to evaluate the impact of temperature on four typical unsaturated soil types. A particle swarm optimization algorithm was employed to calculate the safety factor, ensuring our method’s accuracy by comparing it with existing studies. The results indicate that considering 3D effects yields a higher safety factor, while cracks reduce slope stability. Each unsaturated soil exhibits a distinctive temperature response curve, highlighting the importance of understanding soil types in the design phase.展开更多
Multi-view clustering is a critical research area in computer science aimed at effectively extracting meaningful patterns from complex,high-dimensional data that single-view methods cannot capture.Traditional fuzzy cl...Multi-view clustering is a critical research area in computer science aimed at effectively extracting meaningful patterns from complex,high-dimensional data that single-view methods cannot capture.Traditional fuzzy clustering techniques,such as Fuzzy C-Means(FCM),face significant challenges in handling uncertainty and the dependencies between different views.To overcome these limitations,we introduce a new multi-view fuzzy clustering approach that integrates picture fuzzy sets with a dual-anchor graph method for multi-view data,aiming to enhance clustering accuracy and robustness,termed Multi-view Picture Fuzzy Clustering(MPFC).In particular,the picture fuzzy set theory extends the capability to represent uncertainty by modeling three membership levels:membership degrees,neutral degrees,and refusal degrees.This allows for a more flexible representation of uncertain and conflicting data than traditional fuzzy models.Meanwhile,dual-anchor graphs exploit the similarity relationships between data points and integrate information across views.This combination improves stability,scalability,and robustness when handling noisy and heterogeneous data.Experimental results on several benchmark datasets demonstrate significant improvements in clustering accuracy and efficiency,outperforming traditional methods.Specifically,the MPFC algorithm demonstrates outstanding clustering performance on a variety of datasets,attaining a Purity(PUR)score of 0.6440 and an Accuracy(ACC)score of 0.6213 for the 3 Sources dataset,underscoring its robustness and efficiency.The proposed approach significantly contributes to fields such as pattern recognition,multi-view relational data analysis,and large-scale clustering problems.Future work will focus on extending the method for semi-supervised multi-view clustering,aiming to enhance adaptability,scalability,and performance in real-world applications.展开更多
Federated learning is a machine learning framework designed to protect privacy by keeping training data on clients’devices without sharing private data.It trains a global model through collaboration between clients a...Federated learning is a machine learning framework designed to protect privacy by keeping training data on clients’devices without sharing private data.It trains a global model through collaboration between clients and the server.However,the presence of data heterogeneity can lead to inefficient model training and even reduce the final model’s accuracy and generalization capability.Meanwhile,data scarcity can result in suboptimal cluster distributions for few-shot clients in centralized clustering tasks,and standalone personalization tasks may cause severe overfitting issues.To address these limitations,we introduce a federated learning dual optimization model based on clustering and personalization strategy(FedCPS).FedCPS adopts a decentralized approach,where clients identify their cluster membership locally without relying on a centralized clustering algorithm.Building on this,FedCPS introduces personalized training tasks locally,adding a regularization term to control deviations between local and cluster models.This improves the generalization ability of the final model while mitigating overfitting.The use of weight-sharing techniques also reduces the computational cost of central machines.Experimental results on MNIST,FMNIST,CIFAR10,and CIFAR100 datasets demonstrate that our method achieves better personalization effects compared to other personalized federated learning methods,with an average test accuracy improvement of 0.81%–2.96%.Meanwhile,we adjusted the proportion of few-shot clients to evaluate the impact on accuracy across different methods.The experiments show that FedCPS reduces accuracy by only 0.2%–3.7%,compared to 2.1%–10%for existing methods.Our method demonstrates its advantages across diverse data environments.展开更多
Many fields,such as neuroscience,are experiencing the vast prolife ration of cellular data,underscoring the need fo r organizing and interpreting large datasets.A popular approach partitions data into manageable subse...Many fields,such as neuroscience,are experiencing the vast prolife ration of cellular data,underscoring the need fo r organizing and interpreting large datasets.A popular approach partitions data into manageable subsets via hierarchical clustering,but objective methods to determine the appropriate classification granularity are missing.We recently introduced a technique to systematically identify when to stop subdividing clusters based on the fundamental principle that cells must differ more between than within clusters.Here we present the corresponding protocol to classify cellular datasets by combining datadriven unsupervised hierarchical clustering with statistical testing.These general-purpose functions are applicable to any cellular dataset that can be organized as two-dimensional matrices of numerical values,including molecula r,physiological,and anatomical datasets.We demonstrate the protocol using cellular data from the Janelia MouseLight project to chara cterize morphological aspects of neurons.展开更多
The pursuit of Ag-based alloys with both high strength and toughness has posed a longstanding chal-lenge.In this study,we investigated the cluster strengthening and grain refinement toughening mecha-nisms in fully oxi...The pursuit of Ag-based alloys with both high strength and toughness has posed a longstanding chal-lenge.In this study,we investigated the cluster strengthening and grain refinement toughening mecha-nisms in fully oxidized AgMgNi alloys,which were internally oxidized at 800℃ for 8 h under an oxy-gen atmosphere.We found that Mg-O clusters contributed to the hardening(138 HV)and strengthening(376.9 MPa)of the AgMg alloy through solid solution strengthening effects,albeit at the expense of duc-tility.To address this limitation,we introduced Ni nanoparticles into the AgMg alloy,resulting in signifi-cant grain refinement within its microstructure.Specifically,the grain size decreased from 67.2μm in the oxidized AgMg alloy to below 6.0μm in the oxidized AgMgNi alloy containing 0.3 wt%Ni.Consequently,the toughness increased significantly,rising from toughness value of 2177.9 MJ m^(-3) in the oxidized AgMg alloy to 6186.1 MJ m^(-3) in the oxidized AgMgNi alloy,representing a remarkable 2.8-fold enhancement.Furthermore,the internally oxidized AgMgNi alloy attained a strength of up to 387.6 MPa,comparable to that of the internally oxidized AgMg alloy,thereby demonstrating the successful realization of concurrent strengthening and toughening.These results collectively offer a novel approach for the design of high-performance alloys through the synergistic combination of cluster strengthening and grain refinement toughening.展开更多
Given customizable crystal structure and intriguing optical properties,lanthanide titanium-oxygen clusters(LTOCs)with atomic-level accuracy have gained a lot of interest.In this study,we prepared[Ln_(9)Ti_(2)(μ4-O)(...Given customizable crystal structure and intriguing optical properties,lanthanide titanium-oxygen clusters(LTOCs)with atomic-level accuracy have gained a lot of interest.In this study,we prepared[Ln_(9)Ti_(2)(μ4-O)(μ3-OH)_(14)(acac)_(17)(CH_(3)O)_(2)(CH_(3)OH)_(3)](Ln=Tb_(x)Eu_(9−x)(x=0,4,6,7,8,9),Hacac=acetylacetone),Tb^(3+)and Eu^(3+)co-doped LTOCs,to modify the optical properties for the luminescence thermometer.In detail,the serial LTOCs display dual characteristic emission peaks of ^(5)D_(4)→^(7)F_(5) for Tb^(3+)and^(5)D_(0)→^(7)F_(2) for Eu^(3+)at 548 and 616 nm,respectively,under 330 nm excitation.Effective energy transfer(ET)between Tb^(3+)ions and Eu^(3+)ions was revealed in terms of both emission spectra and luminescence lifetime.The ^(5)D_(0)→^(7)F_(2) emission intensity of Eu^(3+)ions at 616 nm is maximally enhanced(by a factor of 11.2)with a change in the relative molar ratio of Tb^(3+)to Eu^(3+),along with a change in the ET efficiency of Tb^(3+)→Eu^(3+).In addition,the luminescent color changes from red,orange,yellow,to green.This precise control of the ET process between rare-earth ions allows{Tb_(6)Eu_(3)Ti_(2)}to reach a maximum relative sensitivity of 1.241 K^(−1) at 355 K,which is an enhancement of up to 4.6-fold with respect to the previously reported homonuclear emission,holding great potential in the optical thermometers.展开更多
Objectives To identify core symptoms and symptom clusters in patients with neuromyelitis optica spectrum disorder(NMOSD)by network analysis.Methods From October 10 to 30,2023,140 patients with NMOSD were selected to p...Objectives To identify core symptoms and symptom clusters in patients with neuromyelitis optica spectrum disorder(NMOSD)by network analysis.Methods From October 10 to 30,2023,140 patients with NMOSD were selected to participate in this online questionnaire survey.The survey tools included a general information questionnaire and a self-made NMOSD symptoms scale,which included the prevalence,severity,and distress of 29 symptoms.Cluster analysis was used to identify symptom clusters,and network analysis was used to analyze the symptom network and node characteristics and central indicators including strength centrality(r_(s)),closeness centrality(r_(c))and betweeness centrality(r_(b))were used to identify core symptoms and symptom clusters.Results The most common symptom was pain(65.7%),followed by paraesthesia(65.0%),fatigue(65.0%),easy awakening(63.6%).Regarding the burden level of symptoms,pain was the most burdensome symptom,followed by paraesthesia,easy awakening,fatigue,and difficulty falling asleep.Six clusters were identified:somatosensory,motor,visual,and memory symptom clusters,bladder and rectum symptom clusters,sleep symptoms clusters,and neuropsychological symptom clusters.Fatigue(r_(s)=12.39,r_(b)=68.00,r_(c)=0.02)was the most central and prominent bridge symptom,and motor symptom cluster(r_(s)=2.68,r_(c)=0.10)was the most central symptom cluster among the six clusters.Conclusions Our study demonstrated the necessity of symptom management targeting fatigue,pain,and motor symptom cluster in patients with NMOSD.展开更多
High-performance graphite materials have important roles in aerospace and nuclear reactor technologies because of their outstanding chemical stability and high-temperature performance.Their traditional production meth...High-performance graphite materials have important roles in aerospace and nuclear reactor technologies because of their outstanding chemical stability and high-temperature performance.Their traditional production method relies on repeated impregnation-carbonization and graphitization,and is plagued by lengthy preparation cycles and high energy consumption.Phase transition-assisted self-pressurized selfsintering technology can rapidly produce high-strength graphite materials,but the fracture strain of the graphite materials produced is poor.To solve this problem,this study used a two-step sintering method to uniformly introduce micro-nano pores into natural graphite-based bulk graphite,achieving improved fracture strain of the samples without reducing their density and mechanical properties.Using natural graphite powder,micron-diamond,and nano-diamond as raw materials,and by precisely controlling the staged pressure release process,the degree of diamond phase transition expansion was effectively regulated.The strain-to-failure of the graphite samples reached 1.2%,a 35%increase compared to samples produced by fullpressure sintering.Meanwhile,their flexural strength exceeded 110 MPa,and their density was over 1.9 g/cm^(3).The process therefore produced both a high strength and a high fracture strain.The interface evolution and toughening mechanism during the two-step sintering process were investigated.It is believed that the micro-nano pores formed have two roles:as stress concentrators they induce yielding by shear and as multi-crack propagation paths they significantly lengthen the crack propagation path.The two-step sintering phase transition strategy introduces pores and provides a new approach for increasing the fracture strain of brittle materials.展开更多
By systematically reviewing the development status of global carbon dioxide capture,utilization and storage(CCUS)cluster,and comparing domestic and international CCUS industrial models and successful experiences,this ...By systematically reviewing the development status of global carbon dioxide capture,utilization and storage(CCUS)cluster,and comparing domestic and international CCUS industrial models and successful experiences,this study explores the challenges and strategies for the scaled development of the CCUS industry of China.Globally,the CCUS industry has entered a phase of scaled and clustered development.North America has established a system of key technologies in large-scale CO_(2) capture,long-distance pipeline transmission,pipeline network optimization,and large-scale CO_(2) flooding for enhanced oil recovery(CO_(2)-EOR),with relatively mature cluster development and a gradual shift in industrial model from CO_(2)-EOR to geological storage.The CCUS industry of China has developed rapidly across all segments but remains in the early stage of cluster development,facing challenges such as absent business model,insufficient policy support,and technological gaps in core areas.China needs to improve the policy support system to boost enterprises participation across the entire industrial chain,strengthen top-level design and medium-to long-term planning to accelerate demonstration projects construction for whole-process CCUS clusters,advance for a full-chain technological system,including low-cost capture,pipeline optimization and EOR/storage integration technologies,and strengthen personnel training,strengthen discipline construction and university-enterprise research cooperation.展开更多
Thermally activated delayed fluorescence(TADF)materials driven by a through-space charge transfer(TSCT)mechanism have garnered wide interest.However,access of TSCT-TADF molecules with longwavelength emission remains a...Thermally activated delayed fluorescence(TADF)materials driven by a through-space charge transfer(TSCT)mechanism have garnered wide interest.However,access of TSCT-TADF molecules with longwavelength emission remains a formidable challenge.In this study,we introduce a novel V-type DA-D-A’emitter,Trz-mCzCbCz,by using a carborane scaffold.This design strategically incorporates carbazole(Cz)and 2,4,6-triphenyl-1,3,5-triazine(Trz)as donor and acceptor moieties,respectively.Theoretical calculations alongside experimental validations affirm the typical TSCT-TADF characteristics of this luminogen.Owing to the unique structural and electronic attributes of carboranes,Trz-mCzCbCz exhibits an orange-red emission,markedly diverging from the traditional blue-to-green emissions observed in classical Cz and Trz-based TADF molecules.Moreover,bright emission in aggregates was observed for Trz-mCzCbCz with absolute photoluminescence quantum yield(PLQY)of up to 88.8%.As such,we have successfully fabricated five organic light-emitting diodes(OLEDs)by utilizing Trz-mCzCbCz as the emitting layer.It is important to note that both the reverse intersystem crossing process and the TADF properties are profoundly influenced by host materials.The fabricated OLED devices reached a maximum external quantum efficiency(EQE)of 12.7%,with an emission peak at 592 nm.This represents the highest recorded efficiency for TSCT-TADF OLEDs employing carborane derivatives as emitting layers.展开更多
基金The National Science Foundation by Changjiang Scholarship of Ministry of Education of China(No.BCS-0527508)the Joint Research Fund for Overseas Natural Science of China(No.51250110075)+1 种基金the Natural Science Foundation of Jiangsu Province(No.BK200910046)the Postdoctoral Science Foundation of Jiangsu Province(No.0901005C)
文摘In order to analyze the heterogeneity in vehicular traffic speed, a new method that integrates cluster analysis and probability distribution function fitting is presented. First, for identifying the optimal number of clusters, the two-step cluster method is applied to analyze actual speed data, which suggests that dividing speed data into two clusters can best reflect the intrinsic patterns of traffic flows. Such information is then taken as guidance in probability distribution function fitting. The normal, skew-normal and skew-t distribution functions are used to fit the probability distribution of each cluster respectively, which suggests that the skew-t distribution has the highest fitting accuracy; the second is skew-normal distribution; the worst is normal distribution. Model analysis results demonstrate that the proposed mixture model has a better fitting and generalization capability than the conventional single model. In addition, the new method is more flexible in terms of data fitting and can provide a more accurate model of speed distribution.
文摘Under hydrothermal and solvothermal conditions,two novel cobalt-based complexes,{[Co_(2)(CIA)(OH)(1,4-dtb)]·3.2H_(2)O}n(HU23)and{[Co_(2)(CIA)(OH)(1,4-dib)]·3.5H2O·DMF}n(HU24),were successfully constructed by coordinatively assembling the semi-rigid multidentate ligand 5-(1-carboxyethoxy)isophthalic acid(H₃CIA)with the Nheterocyclic ligands 1,4-di(4H-1,2,4-triazol-4-yl)benzene(1,4-dtb)and 1,4-di(1H-imidazol-1-yl)benzene(1,4-dib),respectively,around Co^(2+)ions.Single-crystal X-ray diffraction analysis revealed that in both complexes HU23 and HU24,the CIA^(3-)anions adopt aκ^(7)-coordination mode,bridging six Co^(2+)ions via their five carboxylate oxygen atoms and one ether oxygen atom.This linkage forms tetranuclear[Co4(μ3-OH)2]^(6+)units.These Co-oxo cluster units were interconnected by CIA^(3-)anions to assemble into 2D kgd-type structures featuring a 3,6-connected topology.The 2D layers were further connected by 1,4-dtb and 1,4-dib,resulting in 3D pillar-layered frameworks for HU23 and HU24.Notably,despite the similar configurations of 1,4-dtb and 1,4-dib,differences in their coordination spatial orientations lead to topological divergence in the 3D frameworks of HU23 and HU24.Topological analysis indicates that the frameworks of HU23 and HU24 can be simplified into a 3,10-connected net(point symbol:(4^(10).6^(3).8^(2))(4^(3))_(2))and a 3,8-connected tfz-d net(point symbol:(4^(3))_(2)((4^(6).6^(18).8^(4)))),respectively.This structural differentiation confirms the precise regulatory role of ligands on the topology of metal-organic frameworks.Moreover,the ultraviolet-visible absorption spectra confirmed that HU23 and HU24 have strong absorption capabilities for ultraviolet and visible light.According to the Kubelka-Munk method,their bandwidths were 2.15 and 2.08 eV,respectively,which are consistent with those of typical semiconductor materials.Variable-temperature magnetic susceptibility measurements(2-300 K)revealed significant antiferromagnetic coupling in both complexes,with their effective magnetic moments decreasing markedly as the temperature lowered.CCDC:2457554,HU23;2457553,HU24.
基金supported by the National Natural Science Foundation of China(No.22506042)the Natural Science Foundation of Henan Province(Nos.252300421710 and 252300421552)the High level Talent Research Launch Fund of Henan University of Technology(No.2024BS061).
文摘Effective control of gas-phase pollutants(volatile organic compounds(VOCs)and CO)is critical to human health and the ecological environment.Catalytic oxidation is one of the most promising technologies for achieving efficient volatile organic compounds and CO emission control.The subnano cluster catalyst can not only provide catalytic sites with multiple metal atoms,but also maintain full utilization efficiency.Almost all metal atoms in highly dispersed clusters can be used for adsorption and conversion of reactants.Recently,various types of sub-nano clusters,including subnano cluster oxides,have been developed and demonstrated excellent performance in low-temperature gas-phase pollutants combustion.In this mini review,we systematically summarize the structure,physicochemical properties,characterization,and applications of sub-nano cluster catalysts in catalytic oxidation of CO,methane,propane,propylene,toluene and its derivatives,formaldehyde and chlorinated volatile organic compounds.Finally,we have analyzed and discussed the problems and challenges faced by sub-nano cluster catalysts in both basic research and practical applications,providing a scientific basis for the design,synthesis,and application of efficient heterogeneous catalysts for CO and VOCs oxidation.
基金supported by the Research Project of China Southern Power Grid(No.056200KK52222031).
文摘This paper proposes an equivalent modeling method for photovoltaic(PV)power stations via a particle swarm optimization(PSO)K-means clustering(KMC)algorithm with passive filter parameter clustering to address the complexities,simulation time cost and convergence problems of detailed PV power station models.First,the amplitude–frequency curves of different filter parameters are analyzed.Based on the results,a grouping parameter set for characterizing the external filter characteristics is established.These parameters are further defined as clustering parameters.A single PV inverter model is then established as a prerequisite foundation.The proposed equivalent method combines the global search capability of PSO with the rapid convergence of KMC,effectively overcoming the tendency of KMC to become trapped in local optima.This approach enhances both clustering accuracy and numerical stability when determining equivalence for PV inverter units.Using the proposed clustering method,both a detailed PV power station model and an equivalent model are developed and compared.Simulation and hardwarein-loop(HIL)results based on the equivalent model verify that the equivalent method accurately represents the dynamic characteristics of PVpower stations and adapts well to different operating conditions.The proposed equivalent modeling method provides an effective analysis tool for future renewable energy integration research.
文摘Although k-nearest neighbors （KNN） is a popular fingerprint match algorithm for its simplicity and accuracy, because it is sensitive to the circumstances, a fuzzy c-means （FCM） clustering algorithm is applied to improve it. Thus, a KNN-based two-step FCM weighted （KTFW） algorithm for indoor positioning in wireless local area networks （WLAN） is presented in this paper. In KTFW algorithm, k reference points （RPs） chosen by KNN are clustered through FCM based on received signal strength （RSS） and location coordinates. The right clusters are chosen according to rules, so three sets of RPs are formed including the set of k RPs chosen by KNN and are given different weights. RPs supposed to have better contribution to positioning accuracy are given larger weights to improve the positioning accuracy. Simulation results indicate that KTFW generally outperforms KNN and its complexity is greatly reduced through providing initial clustering centers for FCM.
基金Project supported by the National Key Basic Research Program of China(Grant No.2017YFA0205004)the National Natural Science Foundation of China(Grant Nos.92165201,11474261,and 11634011)+1 种基金the Fundamental Research Funds for the Central Universities(Grant Nos.WK3510000006,and WK3430000003)the Anhui Initiative in Quantum Information Technologies(Grant No.AHY170000)。
文摘Nanoclusters consisting of a few atoms have attracted a lot of research interests due to their exotic size-dependent properties. Here, well-ordered two-dimensional Sb cluster superlattice was fabricated on Si substrate by a two-step method and characterized by scanning tunneling microscopy. High resolution scanning tunneling microscope measurements revealed the fine structures of the Sb clusters, which consist of several Sb atoms ranging from 2 to 7. Furthermore, the electronic structure of the nanocluster displays the quantized energy-level which is due to the single-electron tunneling effects. We believe that the fabrication of Sb cluster superlattice broadens the species of the cluster superlattice and provides a promising candidate to further explore the novel physical and chemical properties of the semimetal nanocluster.
基金supported by the National Natural Science Foun-dation of China(Nos.52025028,52332008,52372214,52202273,and U22A20137)the Priority Academic Program Development(PAPD)of Jiangsu Higher Education Institutions.
文摘Tin(Sn)-lead(Pb)mixed halide perovskites have attracted widespread interest due to their wider re-sponse wavelength and lower toxicity than lead halide perovskites,Among the preparation methods,the two-step method more easily controls the crystallization rate and is suitable for preparing large-area per-ovskite devices.However,the residual low-conductivity iodide layer in the two-step method can affect carrier transport and device stability,and the different crystallization rates of Sn-and Pb-based per-ovskites may result in poor film quality.Therefore,Sn-Pb mixed perovskites are mainly prepared by a one-step method.Herein,a MAPb_(0.5)Sn_(0.5)I_(3)-based self-powered photodetector without a hole transport layer is fabricated by a two-step method.By adjusting the concentration of the ascorbic acid(AA)addi-tive,the final perovskite film exhibited a pure phase without residues,and the optimal device exhibited a high responsivity(0.276 A W^(-1)),large specific detectivity(2.38×10^(12) Jones),and enhanced stability.This enhancement is mainly attributed to the inhibition of Sn2+oxidation,the control of crystal growth,and the sufficient reaction between organic ammonium salts and bottom halides due to the AA-induced pore structure.
文摘Based on DEA - Ridge Regression two-step method, the paper tries to construct industrial cluster competitiveness research framework for empirical analysis, and by the Hunan automobile industry cluster as an example. The study found that Hunan automobile industry cluster competitiveness is relatively weak, full of the very big promotion space; further research shows that the human capital investment, fixed capital investment, land investment and policy support are the main factors influencing the efficiency of automobile industry cluster in Hunan province.
文摘A custom micro-arc oxidation(MAO)apparatus is employed to produce coatings under optimized constant voltage–current two-step power supply mode.Various analytical techniques,including scanning electron microscopy,confocal laser microscopy,X-ray diffraction,X-ray photoelectron spectroscopy,transmission electron microscopy,and electrochemical analysis,are employed to characterize MAO coatings at different stages of preparation.MAO has MgO,hydroxyapatite,Ca_(3)(PO_(4))_(2),and Mg2SiO4 phases.Its microstructure of the coating is characterized by"multiple breakdowns,pores within pores",and"repaired blind pores".The porosity and the uniformity of MAO coating first declines in the constant voltage mode,then augments while the discharge phenomenon takes place,and finally decreases in the repair stage.These analyses reveal a four-stage growth pattern for MAO coatings:anodic oxidation stage,micro-arc oxidation stage,breakdown stage,and repairing stage.During anodic oxidation and MAO stages,inward growth prevails,while the breakdown stage sees outward and accelerated growth.Simultaneous inward and outward growth in the repair stage results in a denser,more uniform coating with increased thickness and improved corrosion resistance.
基金Project(51378510) supported by the National Natural Science Foundation of China。
文摘In existing studies, most slope stability analyses concentrate on conditions with constant temperature, assuming the slope is intact, and employ the Mohr-Coulomb (M-C) failure criterion for saturated soil to characterize the strength of the backfill. However, the actual working temperature of slopes varies, and natural phenomena such as rainfall and groundwater infiltration commonly result in unsaturated soil conditions, with cracks typically present in cohesive slopes. This study introduces a novel approach for assessing the stability of unsaturated soil stepped slopes under varying temperatures, incorporating the effects of open and vertical cracks. Utilizing the kinematic approach and gravity increase method, we developed a three-dimensional (3D) rotational wedge failure mechanism to simulate slope collapse, enhancing the traditional two-dimensional analyses. We integrated temperature-dependent functions and nonlinear shear strength equations to evaluate the impact of temperature on four typical unsaturated soil types. A particle swarm optimization algorithm was employed to calculate the safety factor, ensuring our method’s accuracy by comparing it with existing studies. The results indicate that considering 3D effects yields a higher safety factor, while cracks reduce slope stability. Each unsaturated soil exhibits a distinctive temperature response curve, highlighting the importance of understanding soil types in the design phase.
基金funded by the Research Project:THTETN.05/24-25,VietnamAcademy of Science and Technology.
文摘Multi-view clustering is a critical research area in computer science aimed at effectively extracting meaningful patterns from complex,high-dimensional data that single-view methods cannot capture.Traditional fuzzy clustering techniques,such as Fuzzy C-Means(FCM),face significant challenges in handling uncertainty and the dependencies between different views.To overcome these limitations,we introduce a new multi-view fuzzy clustering approach that integrates picture fuzzy sets with a dual-anchor graph method for multi-view data,aiming to enhance clustering accuracy and robustness,termed Multi-view Picture Fuzzy Clustering(MPFC).In particular,the picture fuzzy set theory extends the capability to represent uncertainty by modeling three membership levels:membership degrees,neutral degrees,and refusal degrees.This allows for a more flexible representation of uncertain and conflicting data than traditional fuzzy models.Meanwhile,dual-anchor graphs exploit the similarity relationships between data points and integrate information across views.This combination improves stability,scalability,and robustness when handling noisy and heterogeneous data.Experimental results on several benchmark datasets demonstrate significant improvements in clustering accuracy and efficiency,outperforming traditional methods.Specifically,the MPFC algorithm demonstrates outstanding clustering performance on a variety of datasets,attaining a Purity(PUR)score of 0.6440 and an Accuracy(ACC)score of 0.6213 for the 3 Sources dataset,underscoring its robustness and efficiency.The proposed approach significantly contributes to fields such as pattern recognition,multi-view relational data analysis,and large-scale clustering problems.Future work will focus on extending the method for semi-supervised multi-view clustering,aiming to enhance adaptability,scalability,and performance in real-world applications.
基金supported by the Foundation of President of Hebei University(XZJJ202303).
文摘Federated learning is a machine learning framework designed to protect privacy by keeping training data on clients’devices without sharing private data.It trains a global model through collaboration between clients and the server.However,the presence of data heterogeneity can lead to inefficient model training and even reduce the final model’s accuracy and generalization capability.Meanwhile,data scarcity can result in suboptimal cluster distributions for few-shot clients in centralized clustering tasks,and standalone personalization tasks may cause severe overfitting issues.To address these limitations,we introduce a federated learning dual optimization model based on clustering and personalization strategy(FedCPS).FedCPS adopts a decentralized approach,where clients identify their cluster membership locally without relying on a centralized clustering algorithm.Building on this,FedCPS introduces personalized training tasks locally,adding a regularization term to control deviations between local and cluster models.This improves the generalization ability of the final model while mitigating overfitting.The use of weight-sharing techniques also reduces the computational cost of central machines.Experimental results on MNIST,FMNIST,CIFAR10,and CIFAR100 datasets demonstrate that our method achieves better personalization effects compared to other personalized federated learning methods,with an average test accuracy improvement of 0.81%–2.96%.Meanwhile,we adjusted the proportion of few-shot clients to evaluate the impact on accuracy across different methods.The experiments show that FedCPS reduces accuracy by only 0.2%–3.7%,compared to 2.1%–10%for existing methods.Our method demonstrates its advantages across diverse data environments.
基金supported in part by NIH grants R01NS39600,U01MH114829RF1MH128693(to GAA)。
文摘Many fields,such as neuroscience,are experiencing the vast prolife ration of cellular data,underscoring the need fo r organizing and interpreting large datasets.A popular approach partitions data into manageable subsets via hierarchical clustering,but objective methods to determine the appropriate classification granularity are missing.We recently introduced a technique to systematically identify when to stop subdividing clusters based on the fundamental principle that cells must differ more between than within clusters.Here we present the corresponding protocol to classify cellular datasets by combining datadriven unsupervised hierarchical clustering with statistical testing.These general-purpose functions are applicable to any cellular dataset that can be organized as two-dimensional matrices of numerical values,including molecula r,physiological,and anatomical datasets.We demonstrate the protocol using cellular data from the Janelia MouseLight project to chara cterize morphological aspects of neurons.
基金supported by the National Natural Science Foundation of China(Nos.51977027 and 51967008)the Scientific and Technological Project of Yunnan Precious Metals Lab-oratory(Nos.YPML-2023050250 and YPML-2022050206).
文摘The pursuit of Ag-based alloys with both high strength and toughness has posed a longstanding chal-lenge.In this study,we investigated the cluster strengthening and grain refinement toughening mecha-nisms in fully oxidized AgMgNi alloys,which were internally oxidized at 800℃ for 8 h under an oxy-gen atmosphere.We found that Mg-O clusters contributed to the hardening(138 HV)and strengthening(376.9 MPa)of the AgMg alloy through solid solution strengthening effects,albeit at the expense of duc-tility.To address this limitation,we introduced Ni nanoparticles into the AgMg alloy,resulting in signifi-cant grain refinement within its microstructure.Specifically,the grain size decreased from 67.2μm in the oxidized AgMg alloy to below 6.0μm in the oxidized AgMgNi alloy containing 0.3 wt%Ni.Consequently,the toughness increased significantly,rising from toughness value of 2177.9 MJ m^(-3) in the oxidized AgMg alloy to 6186.1 MJ m^(-3) in the oxidized AgMgNi alloy,representing a remarkable 2.8-fold enhancement.Furthermore,the internally oxidized AgMgNi alloy attained a strength of up to 387.6 MPa,comparable to that of the internally oxidized AgMg alloy,thereby demonstrating the successful realization of concurrent strengthening and toughening.These results collectively offer a novel approach for the design of high-performance alloys through the synergistic combination of cluster strengthening and grain refinement toughening.
基金supported by the National Natural Science Foundation of China(Nos.12174151 and 12304448)the Specific Research Fund of the Innovation Platform for Academicians of Hainan Province(No.YSPTZX202208)+3 种基金Hainan Province Clinical Medical Center(No.QWYH_(2)022341)the Key Laboratory of New Energy and Rare Earth Resource Utilization of the State People’s Committee of China(No.NERE202206)the Department of Science and Technology of Jilin Province(No.20220101059JC)the Key Laboratory of the Ministry of Education for First Aid and Trauma Research(No.KLET-202218).
文摘Given customizable crystal structure and intriguing optical properties,lanthanide titanium-oxygen clusters(LTOCs)with atomic-level accuracy have gained a lot of interest.In this study,we prepared[Ln_(9)Ti_(2)(μ4-O)(μ3-OH)_(14)(acac)_(17)(CH_(3)O)_(2)(CH_(3)OH)_(3)](Ln=Tb_(x)Eu_(9−x)(x=0,4,6,7,8,9),Hacac=acetylacetone),Tb^(3+)and Eu^(3+)co-doped LTOCs,to modify the optical properties for the luminescence thermometer.In detail,the serial LTOCs display dual characteristic emission peaks of ^(5)D_(4)→^(7)F_(5) for Tb^(3+)and^(5)D_(0)→^(7)F_(2) for Eu^(3+)at 548 and 616 nm,respectively,under 330 nm excitation.Effective energy transfer(ET)between Tb^(3+)ions and Eu^(3+)ions was revealed in terms of both emission spectra and luminescence lifetime.The ^(5)D_(0)→^(7)F_(2) emission intensity of Eu^(3+)ions at 616 nm is maximally enhanced(by a factor of 11.2)with a change in the relative molar ratio of Tb^(3+)to Eu^(3+),along with a change in the ET efficiency of Tb^(3+)→Eu^(3+).In addition,the luminescent color changes from red,orange,yellow,to green.This precise control of the ET process between rare-earth ions allows{Tb_(6)Eu_(3)Ti_(2)}to reach a maximum relative sensitivity of 1.241 K^(−1) at 355 K,which is an enhancement of up to 4.6-fold with respect to the previously reported homonuclear emission,holding great potential in the optical thermometers.
基金supported by the Specific Research Fund for Top-notch Talents of Guangdong Provincial Hospital of Chinese Medicine(No.2022KT1188).
文摘Objectives To identify core symptoms and symptom clusters in patients with neuromyelitis optica spectrum disorder(NMOSD)by network analysis.Methods From October 10 to 30,2023,140 patients with NMOSD were selected to participate in this online questionnaire survey.The survey tools included a general information questionnaire and a self-made NMOSD symptoms scale,which included the prevalence,severity,and distress of 29 symptoms.Cluster analysis was used to identify symptom clusters,and network analysis was used to analyze the symptom network and node characteristics and central indicators including strength centrality(r_(s)),closeness centrality(r_(c))and betweeness centrality(r_(b))were used to identify core symptoms and symptom clusters.Results The most common symptom was pain(65.7%),followed by paraesthesia(65.0%),fatigue(65.0%),easy awakening(63.6%).Regarding the burden level of symptoms,pain was the most burdensome symptom,followed by paraesthesia,easy awakening,fatigue,and difficulty falling asleep.Six clusters were identified:somatosensory,motor,visual,and memory symptom clusters,bladder and rectum symptom clusters,sleep symptoms clusters,and neuropsychological symptom clusters.Fatigue(r_(s)=12.39,r_(b)=68.00,r_(c)=0.02)was the most central and prominent bridge symptom,and motor symptom cluster(r_(s)=2.68,r_(c)=0.10)was the most central symptom cluster among the six clusters.Conclusions Our study demonstrated the necessity of symptom management targeting fatigue,pain,and motor symptom cluster in patients with NMOSD.
基金Natural Science Foundation of Shanghai(24ZR1400800)he Natural Science Foundation of China(U23A20685,52073058,91963204)+1 种基金the National Key R&D Program of China(2021YFB3701400)Shanghai Sailing Program(23YF1400200)。
文摘High-performance graphite materials have important roles in aerospace and nuclear reactor technologies because of their outstanding chemical stability and high-temperature performance.Their traditional production method relies on repeated impregnation-carbonization and graphitization,and is plagued by lengthy preparation cycles and high energy consumption.Phase transition-assisted self-pressurized selfsintering technology can rapidly produce high-strength graphite materials,but the fracture strain of the graphite materials produced is poor.To solve this problem,this study used a two-step sintering method to uniformly introduce micro-nano pores into natural graphite-based bulk graphite,achieving improved fracture strain of the samples without reducing their density and mechanical properties.Using natural graphite powder,micron-diamond,and nano-diamond as raw materials,and by precisely controlling the staged pressure release process,the degree of diamond phase transition expansion was effectively regulated.The strain-to-failure of the graphite samples reached 1.2%,a 35%increase compared to samples produced by fullpressure sintering.Meanwhile,their flexural strength exceeded 110 MPa,and their density was over 1.9 g/cm^(3).The process therefore produced both a high strength and a high fracture strain.The interface evolution and toughening mechanism during the two-step sintering process were investigated.It is believed that the micro-nano pores formed have two roles:as stress concentrators they induce yielding by shear and as multi-crack propagation paths they significantly lengthen the crack propagation path.The two-step sintering phase transition strategy introduces pores and provides a new approach for increasing the fracture strain of brittle materials.
基金Supported by the PetroChina Science and Technology Major Project(2021ZZ01-05)Hainan Merit-based Recruitment Project(ZDYF2024SHFZ147)National Natural Science Foundation of China(NNSC)Project(52474033)。
文摘By systematically reviewing the development status of global carbon dioxide capture,utilization and storage(CCUS)cluster,and comparing domestic and international CCUS industrial models and successful experiences,this study explores the challenges and strategies for the scaled development of the CCUS industry of China.Globally,the CCUS industry has entered a phase of scaled and clustered development.North America has established a system of key technologies in large-scale CO_(2) capture,long-distance pipeline transmission,pipeline network optimization,and large-scale CO_(2) flooding for enhanced oil recovery(CO_(2)-EOR),with relatively mature cluster development and a gradual shift in industrial model from CO_(2)-EOR to geological storage.The CCUS industry of China has developed rapidly across all segments but remains in the early stage of cluster development,facing challenges such as absent business model,insufficient policy support,and technological gaps in core areas.China needs to improve the policy support system to boost enterprises participation across the entire industrial chain,strengthen top-level design and medium-to long-term planning to accelerate demonstration projects construction for whole-process CCUS clusters,advance for a full-chain technological system,including low-cost capture,pipeline optimization and EOR/storage integration technologies,and strengthen personnel training,strengthen discipline construction and university-enterprise research cooperation.
基金supported by the Natural Science Foundation of Jiangsu Province(No.BZ2022007)the National Natural Science Foundation of China(No.92261202)+1 种基金the Ministry of Science and Technology of the People’s Republic of China(No.2021YFE0114800)the Ministry of Science and Higher Education of the Russian Federation(No.075-15-2021-1027).
文摘Thermally activated delayed fluorescence(TADF)materials driven by a through-space charge transfer(TSCT)mechanism have garnered wide interest.However,access of TSCT-TADF molecules with longwavelength emission remains a formidable challenge.In this study,we introduce a novel V-type DA-D-A’emitter,Trz-mCzCbCz,by using a carborane scaffold.This design strategically incorporates carbazole(Cz)and 2,4,6-triphenyl-1,3,5-triazine(Trz)as donor and acceptor moieties,respectively.Theoretical calculations alongside experimental validations affirm the typical TSCT-TADF characteristics of this luminogen.Owing to the unique structural and electronic attributes of carboranes,Trz-mCzCbCz exhibits an orange-red emission,markedly diverging from the traditional blue-to-green emissions observed in classical Cz and Trz-based TADF molecules.Moreover,bright emission in aggregates was observed for Trz-mCzCbCz with absolute photoluminescence quantum yield(PLQY)of up to 88.8%.As such,we have successfully fabricated five organic light-emitting diodes(OLEDs)by utilizing Trz-mCzCbCz as the emitting layer.It is important to note that both the reverse intersystem crossing process and the TADF properties are profoundly influenced by host materials.The fabricated OLED devices reached a maximum external quantum efficiency(EQE)of 12.7%,with an emission peak at 592 nm.This represents the highest recorded efficiency for TSCT-TADF OLEDs employing carborane derivatives as emitting layers.
