When the radio frequency identification(RFID)system inventories multiple tags,the recognition rate will be seriously affected due to collisions.Based on the existing dynamic frame slotted Aloha(DFSA)algorithm,a sub-fr...When the radio frequency identification(RFID)system inventories multiple tags,the recognition rate will be seriously affected due to collisions.Based on the existing dynamic frame slotted Aloha(DFSA)algorithm,a sub-frame observation and cyclic redundancy check(CRC)grouping combined dynamic framed slotted Aloha(SUBF-CGDFSA)algorithm is proposed.The algorithm combines the precise estimation method of the quantity of large-scale tags,the large-scale tags grouping mechanism based on CRC pseudo-randomcharacteristics,and the Aloha anti-collision optimization mechanism based on sub-frame observation.By grouping tags and sequentially identifying themwithin subframes,it accurately estimates the number of remaining tags and optimizes frame length accordingly to improve efficiency in large-scale RFID systems.Simulation outcomes demonstrate that this proposed algorithmcan effectively break through the system throughput bottleneck of 36.8%,which is up to 30%higher than the existing DFSA standard scheme,and has more significant advantages,which is suitable for application in largescale RFID tags scenarios.展开更多
Addressing the challenges of passive Radio Frequency Identification(RFID)indoor localization technology in Non-Line-of-Sight(NLoS)and multipath environments,this paper presents an innovative approach by introducing a ...Addressing the challenges of passive Radio Frequency Identification(RFID)indoor localization technology in Non-Line-of-Sight(NLoS)and multipath environments,this paper presents an innovative approach by introducing a combined technology integrating an improved Kalman Filter with Space Domain Phase Difference of Arrival(SD-PDOA)and Received Signal Strength Indicator(RSSI).This methodology utilizes the distinct channel characteristics in multipath and NLoS contexts to effectively filter out interference and accurately extract localization information,thereby facilitating high precision and stability in passive RFID localization.The efficacy of this approach is demonstrated through detailed simulations and empirical tests conducted on a custom-built experimental platform consisting of passive RFID tags and an R420 reader.The findings are significant:in NLoS conditions,the four-antenna localization system achieved a notable localization accuracy of 0.25 m at a distance of 5 m.In complex multipath environments,this system achieved a localization accuracy of approximately 0.5 m at a distance of 5 m.When compared to conventional passive localization methods,our proposed solution exhibits a substantial improvement in indoor localization accuracy under NLoS and multipath conditions.This research provides a robust and effective technical solution for high-precision passive indoor localization in the Internet of Things(IoT)system,marking a significant advancement in the field.展开更多
Studying user electricity consumption behavior is crucial for understanding their power usage patterns.However,the traditional clustering methods fail to identify emerging types of electricity consumption behavior.To ...Studying user electricity consumption behavior is crucial for understanding their power usage patterns.However,the traditional clustering methods fail to identify emerging types of electricity consumption behavior.To address this issue,this paper introduces a statistical analysis of clusters and evaluates the set of indicators for power usage patterns.The fuzzy C-means clustering algorithm is then used to analyze 6 months of electricity consumption data in 2017 from energy storage equipment,agricultural drainage irrigation,port shore power,and electric vehicles.Finally,the proposed method is validated through experiments,where the Davies-Bouldin index and profile coefficient are calculated and compared.Experiments showed that the optimal number of clusters is 4.This study demonstrates the potential of using a fuzzy C-means clustering algorithmin identifying emerging types of electricity consumption behavior,which can help power system operators and policymakers to make informed decisions and improve energy efficiency.展开更多
The kinetic behavior of esterification between methacrylic acid and methanol catalyzed by NKC-9 resin was studied in a fixed bed reactor.The reaction was conducted in the temperature range of 323.15 to 368.15 K with t...The kinetic behavior of esterification between methacrylic acid and methanol catalyzed by NKC-9 resin was studied in a fixed bed reactor.The reaction was conducted in the temperature range of 323.15 to 368.15 K with the molar ratio of reactants from 0.8 to 1.4 under certain pressure.The measurement data were regression with the pseudo-homogeneous(P-H),Eley-Rideal(E-R),and Langmuir-Hinshelwood(L-H)heterogeneous kinetic models.Independent adsorption experiments were implemented to gain the adsorption equilibrium constants of four components.Among the above three models,the L-H model exhibited the best fitting results.The stability of NKC-9 was evaluated by long-term running with the yield of methyl methacrylate no decrease during 3000 h operation.The structure and physicochemical properties of the new and used catalyst were performed by several characterizations including thermogravimetric analysis(TG),scanning electron microscope(SEM),X-ray diffraction(XRD)and Fourier transform infrared spectroscopy(FT-IR)and so on.展开更多
Developments in advanced manufacturing have promoted the miniaturization of semiconductor electronic devices to a near-atomic scale,which continuously follows the‘top-down’construction method.However,huge challenges...Developments in advanced manufacturing have promoted the miniaturization of semiconductor electronic devices to a near-atomic scale,which continuously follows the‘top-down’construction method.However,huge challenges have been encountered with the exponentially increased cost and inevitably prominent quantum effects.Molecular electronics is a highly interdisciplinary subject that studies the quantum behavior of electrons tunneling in molecules.It aims to assemble electronic devices in a‘bottom-up’manner on this scale through a single molecule,thereby shedding light on the future design of logic circuits with new operating principles.The core technologies in this field are based on the rapid development of precise fabrication at a molecular scale,regulation at a quantum scale,and related applications of the basic electronic component of the‘electrode-molecule-electrode junction’.Therefore,the quantum charge transport properties of the molecule can be controlled to pave the way for the bottom-up construction of single-molecule devices.The review firstly focuses on the collection and classification of the construction methods for molecular junctions.Thereafter,various characterization and regulation methods for molecular junctions are discussed,followed by the properties based on tunneling theory at the quantum scale of the corresponding molecular electronic devices.Finally,a summary and perspective are given to discuss further challenges and opportunities for the future design of electronic devices.展开更多
We report a rare case of intratumoral hemorrhage during postoperative radiotherapy for pituitary adenoma. A 57-year-old Asian male, complaining of long-standing eye strain, underwent a medical checkup of the brain. Ma...We report a rare case of intratumoral hemorrhage during postoperative radiotherapy for pituitary adenoma. A 57-year-old Asian male, complaining of long-standing eye strain, underwent a medical checkup of the brain. Magnetic resonance imaging showed a multicystic giant pituitary adenoma. The patient underwent an endoscopic endonasal transsphenoidal partial removal of the adenoma to provide optic pathway decompression and got relief from the visual symptoms. Just before completion of the postoperative radiotherapy for residual adenoma, the patient developed right hemiparesis, mild motor aphasia, and right oculomotor palsy. A cranial CT scan showed intratumoral hemorrhage into the intratumoral cyst. The patient therefore had to undergo three additional craniotomies for evacuation of cyst contents over the next 8 months. The follow-up MRI at 11 months after the initial hemorrhage showed that the new oozing of blood in the intratumoral cyst was still appearing. Intratumoral hemorrhage is a rare, albeit life-threatening, complication of pituitary adenoma. We reviewed relevant literature and suggested that the cystic component in pituitary adenoma could be a key pathogenesis of this rare complication. In conclusion, we suggest that it may be necessary to realize that cases which have cystic giant pituitary adenoma may cause hemorrhage by chance with the foreseeability.展开更多
Metallic clusters,ranging from 1 to 2 nm in size,have emerged as promising candidates for creating nanoelectronic devices at the single-cluster level.With the intermediate quantum properties between metals and semicon...Metallic clusters,ranging from 1 to 2 nm in size,have emerged as promising candidates for creating nanoelectronic devices at the single-cluster level.With the intermediate quantum properties between metals and semiconductors,these metallic clusters offer an alternative pathway to silicon-based electronics and organic molecules for miniaturized electronics with dimensions below 5 nm.Significant progress has been made in studies of single-cluster electronic devices.However,a clear guide for selecting,synthesizing,and fabricating functional single-cluster electronic devices is still required.This review article provides a comprehensive overview of single-cluster electronic devices,including the mechanisms of electron transport,the fabrication of devices,and the regulations of electron transport properties.Furthermore,we discuss the challenges and future directions for single-cluster electronic devices and their potential applications.展开更多
Charge transport characterization of single-molecule junctions is essential for the fundamental research of single-molecule physical chemistry and the development towards single-molecule electronic devices and circuit...Charge transport characterization of single-molecule junctions is essential for the fundamental research of single-molecule physical chemistry and the development towards single-molecule electronic devices and circuits. Among the single-molecule conductance characterization techniques,the single-molecule break junction technique is widely used in tens of worldwide research laboratories which can generate a large amount of experimental data from thousands of individual measurement cycles. However,data interpretation is a challenging task for researchers with different research backgrounds,and the different data analysis approaches sometimes lead to the misunderstanding of the measurement data and even reproducibility issues of the measurement. It is thus a necessity to develop a user-friendly all-in-one data analysis tool that automatizes the basic data analysis in a standard and widely accepted way. In this work,we present the XMe Code (Xiamen Molecular Electronics Code),an intelligent all-in-one data analysis tool for the comprehensive analysis of single-molecule break junction data. XMe code provides end-to-end data analysis that takes in the original experimental data and returns electronic characteristics and even charge transport mechanisms. We believe that XMe Code will promote the transparency of the data analysis in single-molecule electronics and the collaborations among scientists with different research backgrounds.展开更多
Cardiac biological pacing(BP)is one of the future directions for bradyarrhythmias intervention.Currently,cardiac pacemaker cells(PCs)used for cardiac BP are mainly derived from pluripotent stem cells(PSCs).However,the...Cardiac biological pacing(BP)is one of the future directions for bradyarrhythmias intervention.Currently,cardiac pacemaker cells(PCs)used for cardiac BP are mainly derived from pluripotent stem cells(PSCs).However,the production of high-quality cardiac PCs from PSCs remains a challenge.Here,we developed a cardiac PC differentiation strategy by adopting dual PC markers and simulating the developmental route of PCs.First,two PC markers,Shox2 and Hcn4,were selected to establish Shox2:EGFP;Hcn4:mCherry mouse PSC reporter line.Then,by stepwise guiding naïve PSCs to cardiac PCs following naïve to formative pluripotency transition and manipulating signaling pathways during cardiac PCs differentiation,we designed the FSK method that increased the yield of SHOX2^(+);HCN4^(+)cells with typical PC characteristics,which was 12 and 42 folds higher than that of the embryoid body(EB)and the monolayer M10 methods respectively.In addition,the in vitro cardiac PCs differentiation trajectory was mapped by single-cell RNA sequencing(scRNA-seq),which resembled in vivo PCs development,and ZFP503 was verified as a key regulator of cardiac PCs differentiation.These PSC-derived cardiac PCs have the potential to drive advances in cardiac BP technology,help with the understanding of PCs(patho)physiology,and benefit drug discovery for PC-related diseases as well.展开更多
Spiropyran derivatives are prototype mechanophores with a promising application as molecular sensors because of their changeable structure under external force stimuli.However,the chemical structure evolution under ex...Spiropyran derivatives are prototype mechanophores with a promising application as molecular sensors because of their changeable structure under external force stimuli.However,the chemical structure evolution under external stimuli remains unclear due to the uncertainty and difficulty in distinguishing the structures of different ring-opened merocyanine isomers generated in the force-induced reaction.Here we identify the structure of isomers produced by the force-induced reaction of spiropyran derivatives using a single-molecule conductance measurement and an unsupervised clustering algorithm.We found that the original data from the single-molecule conductance measurement can be divided into four clusters through unsupervised clustering.By introducing a photoinduced reaction and theoretical calculation,we identified and attributed the four clusters of data to the multiple states of the molecular junctions.Our work demonstrates that a single-molecule break junction measurement can distinguish the isomers in the force-induced reaction,suggesting the great potential of single-molecule conductance measurement and unsupervised clustering approaches for structural analysis.展开更多
Sorting out organic molecules with high thermopower is essential for understanding molecular thermoelectrics.The intermolecular coupling offers a unique chance to enhance the thermopower by tuning the bandgap structur...Sorting out organic molecules with high thermopower is essential for understanding molecular thermoelectrics.The intermolecular coupling offers a unique chance to enhance the thermopower by tuning the bandgap structure of molecular devices,but the investigation of intermolecular coupling in bulk materials remains challenging.Herein,we investigated the thermopower of diketopyrrolopyrrole(DPP)cored single-molecule junctions with different coupling strengths by varying the packing density of the self-assembled monolayers(SAM)using a customized scanning tunneling microscope break junction(STM-BJ)technique.We found that the thermopower of DPP molecules could be enhanced up to one order of magnitude with increasing packing density,suggesting that the thermopower increases with larger neighboring intermolecular interactions.The combined density functional theory(DFT)calculations revealed that the closely-packed configuration brings stronger intermolecular coupling and then reduces the highest occupied molecular orbital(HOMO)-lowest unoccupied molecular orbital(LUMO)gap,leading to an enhanced thermopower.Our findings offer a new strategy for developing organic thermoelectric devices with high thermopower.展开更多
Many cyclobutane natural products have intriguing biological properties that arise from their fascinating chemical structures.Cyclobutane natural products feature a cyclobutane scaffold as the core or as a part of the...Many cyclobutane natural products have intriguing biological properties that arise from their fascinating chemical structures.Cyclobutane natural products feature a cyclobutane scaffold as the core or as a part of the spirocyclic or fused cyclic core.However,the highly functionalized nature and the inherent stereochemistry of these cyclobutane natural products,which are associated with their biological activities,pose tremendous challenges to their preparation.In this perspective,we present contemporary advancements in synthetic methods and/or strategies en route to the bioactive cyclobutane natural products.We begin by describing the representative bioactive cyclobutane natural products and then focus on illustrative examples of their syntheses reported from 2018 to 2021.These advances will enable efficient syntheses of cyclobutanes of structural and biological importance.展开更多
We report an electrochemically assisted mechanically controllable break junction (EC-MCBJ) approach to investigating single molecule conductance. Electrode pairs connected with a gold nanobridge were fabricated by e...We report an electrochemically assisted mechanically controllable break junction (EC-MCBJ) approach to investigating single molecule conductance. Electrode pairs connected with a gold nanobridge were fabricated by electrochemical deposition and then mounted on a homebuilt MCBJ platform. A large number of Au- molecule-Au junctions were produced sequentially by repeated breaking and reconnecting of the gold nanobridge. In order to measure their single molecule conductance, statistical conductance histograms were generated for benzene-l,4-dithiol (BDT) and 4,4'-bipyridine (BPY). The values extracted from these histograms were found to be in the same range as values previously reported in the literature. Our method is distinct from the ones used to acquire these previously reported literature values, however, in that it is faster, simpler, more cost-effective, and changing the electrode material is more convenient.展开更多
Benefiting from the development of molecular electronics and molecular plasmonics, the interplay of light and electronic transport in molecular junctions has attracted growing interest among researchers in both fields...Benefiting from the development of molecular electronics and molecular plasmonics, the interplay of light and electronic transport in molecular junctions has attracted growing interest among researchers in both fields, leading to a new research direction of "single-molecule optoelectronics". Here, we review the latest developments of photo-modulated charge transport,electroluminescence and Raman spectroscopy from single-molecule junctions, and suggest future directions for single-molecule optoelectronics.展开更多
In this article, we report on the fabrication and transport measurements of Cu quantum point contacts prepared by a novel, electrochemically assisted mechanically controllable break junction (EC-MCBJ) method. By emp...In this article, we report on the fabrication and transport measurements of Cu quantum point contacts prepared by a novel, electrochemically assisted mechanically controllable break junction (EC-MCBJ) method. By employing photolithography and wet-etching processes, suspended electrode pairs were patterned and fabricated successfully on Si microchips. Rather than adopting an acid Cu electroplating solution, a novel alkaline electroplating solution was developed and utilized to establish Cu nanocontacts between electrode pairs. Typically, the widths of the as-fabricated Cu nanocontacts were found to be smaller than 18 nm. A large number of Cu quantum point contacts were then produced and characterized by a home-built MCBJ setup. In addition to the conventional histogram, where peaks tend to decrease in amplitude with increasing conductance, an anomalous type of conductance histogram, exhibiting different peak amplitudes, was observed. Through statistical analysis of the maximum allowable bending of the Si microchips, and theoretical calculations, we demonstrated that our alkaline Cu electroplating solution affords Cu nanocontacts that are compatible with subsequent MCBJ operations, which is essential for the fabrication of Cu quantum point contacts. As sophisticated e-beam lithography is not required, the EC-MCBJ method is fast, simple, and cost-effective. Moreover, it is likely to be suitable for the fabrication and characterization of quantum point contacts of various metals from their respective electroplating solutions.展开更多
In this article, we report on the characterization of various molecular junctions' current-voltage characteristics (Ⅰ-Ⅴ curves) evolution under mechanical modulations, by employing a novel electrochemically assis...In this article, we report on the characterization of various molecular junctions' current-voltage characteristics (Ⅰ-Ⅴ curves) evolution under mechanical modulations, by employing a novel electrochemically assisted-mechanically controllable break junction (EC-MCBJ) method. For 1,4-benzenedithiol, the Ⅰ-Ⅴ curves measured at constant electrode pair separation show excellent reproducibility, indicating the feasibility of our EC-MCBJ method for fabricating molecular junctions. For ferrocene-bisvinylphenylmethyl dithiol (Fc-VPM), an anomalous type of Ⅰ-Ⅴ curve was observed by the particular control over the stepping motor. This phenomenon is rationalized assuming a model of atomic contact evolution with the presence of molecular junctions. To test this hypothesized model, a molecule with a longer length, 1,3-butadiyne-linked dinuclear ruthenium(H) complex (Ru-1), was implemented, and the Ⅰ-Ⅴ curve evolution was investigated under similar circumstances. Compared with Fc-VPM, the observed Ⅰ-Ⅴ curves show close analogy and minor differences, and both of them fit the hypothesized model well.展开更多
Molecular rectifier, as a basic function of molecular electronic devices, has attracted extensive attention for the opportunity in constructing sub-nanometer electronic devices. However, tunneling leakage current has ...Molecular rectifier, as a basic function of molecular electronic devices, has attracted extensive attention for the opportunity in constructing sub-nanometer electronic devices. However, tunneling leakage current has a significant contribution as electronic devices shrink in size, which leads to a challenge in fabricating molecular rectifiers at the sub-nanometer scale. Here, we experimentally demonstrate a sub-nanometer molecular rectifier based on the supramolecular junction assembled between water and 1,4-diazabicyclo[2.2.2]octane (DABCO) molecule. The charge transport through DABCO and corresponding supramolecular junctions exhibits destructive σ-interference, ensuring a sharp conductance variation for transmission modulation. The supramolecular interaction between DABCO and water readily introduces the asymmetric electrode-molecule interaction, which combines with the destructive σ-interference to support the sub-nanometer rectification.展开更多
The conductance through single-molecule junctions characterized by the break junction techniques consists of the through-space tunneling and through-molecule tunneling conductance, and the existence of through-space t...The conductance through single-molecule junctions characterized by the break junction techniques consists of the through-space tunneling and through-molecule tunneling conductance, and the existence of through-space tunneling between the electrodes makes the quantitative extraction of the intrinsic molecular signals of single-molecule junctions challenging. Here, we established an analytic model to describe the evolution of the conductance of a single molecule in break junction measurements. The experimental data for a series of oligo(aryleneethynylene) derivatives validate the proposed model, which provides a modeling insight into the conductance evolution for the opening process in a "real" break junction experiment. Further modulations revealed that the junction formation probability and rupture distance of the molecular junction, which reflect the junction stability, will significantly influence the amplitude and position of the obtained conductance peak. We further extend our model to a diffusion and a chemical reaction process, for which the simulation results show that the break junction technique offers a quantitative understanding of these time-dependent systems, suggesting the potential of break junction techniques in the quantitative characterization of physical and chemical processes at the single-molecule scale.展开更多
The investigation of electronic excited states in single-molecule junctions not only provides platforms to reveal the photophysical and photochemical processes at the molecular level,but also brings opportunities for ...The investigation of electronic excited states in single-molecule junctions not only provides platforms to reveal the photophysical and photochemical processes at the molecular level,but also brings opportunities for the development of single-molecule optoelectronic devices.Understanding the interaction mechanisms between molecules and nanocavities is essential to obtain ondemand properties in devices by artificial design,since molecules in junctions exhibit unique behaviors of excited states benefited from the structures of metallic nanocavities.Here,we review the excitation mechanisms involved in the interplay between molecules and plasmonic nanocavities,and reveal the influence of nanostructures on excited-state properties by demonstrating the differences in excited state decay processes.Furthermore,vibronic transitions of molecules between nanoelectrodes are also discussed,offering a new single-molecule characterization method.Finally,we provide the potential applications and challenges in single-molecule optoelectronic devices and the possible directions in exploring the underlying mechanisms of photophysical and photochemical processes.展开更多
The quantum interference effect in the charge transport through single-phenyl molecules received intensive interests from theory but remained as an experimental challenge. In this paper, we investigated the charge tra...The quantum interference effect in the charge transport through single-phenyl molecules received intensive interests from theory but remained as an experimental challenge. In this paper, we investigated the charge transport through single-molecule benzene dithiol (BDT) junction with different connectivities using mechanically controllable break.junction (MCB]) technique. By further improving the mechanical stability and the electronic measuring component of the MCBJ set-up, we obtained the conductance histograms of BDT molecules (BDTs) from the statistical analysis of conductance-distance traces without data selection. By tuning the connectivity, the conductance of BDTs is determined to be 10-12Go, 10-22Go and 10-10Go for pcra, meta, and ortho connectivity, following the trend that ortfio-BDT 〉 para-BDT 〉 meta-BDT. Furthermore, the displacements of the junctions followed the trend that para 〉 meta 〉 ortho, suggesting the charge transport through the molecules via the gold-thiol bond. The different trends between conductance and displacement for different connectivities suggests the presence of destructive quantum interference effect on meta-BDT, which provides the experimental evidence for the quantum interference effect through single-phenyl molecular junctions.展开更多
基金supported in part by National Natural Science Foundation of China(U22B2004,62371106)in part by the Joint Project of China Mobile Research Institute&X-NET(Project Number:2022H002)+6 种基金in part by the Pre-Research Project(31513070501)in part by National Key R&D Program(2018AAA0103203)in part by Guangdong Provincial Research and Development Plan in Key Areas(2019B010141001)in part by Sichuan Provincial Science and Technology Planning Program of China(2022YFG0230,2023YFG0040)in part by the Fundamental Enhancement Program Technology Area Fund(2021-JCJQ-JJ-0667)in part by the Joint Fund of ZF and Ministry of Education(8091B022126)in part by Innovation Ability Construction Project for Sichuan Provincial Engineering Research Center of Communication Technology for Intelligent IoT(2303-510109-04-03-318020).
文摘When the radio frequency identification(RFID)system inventories multiple tags,the recognition rate will be seriously affected due to collisions.Based on the existing dynamic frame slotted Aloha(DFSA)algorithm,a sub-frame observation and cyclic redundancy check(CRC)grouping combined dynamic framed slotted Aloha(SUBF-CGDFSA)algorithm is proposed.The algorithm combines the precise estimation method of the quantity of large-scale tags,the large-scale tags grouping mechanism based on CRC pseudo-randomcharacteristics,and the Aloha anti-collision optimization mechanism based on sub-frame observation.By grouping tags and sequentially identifying themwithin subframes,it accurately estimates the number of remaining tags and optimizes frame length accordingly to improve efficiency in large-scale RFID systems.Simulation outcomes demonstrate that this proposed algorithmcan effectively break through the system throughput bottleneck of 36.8%,which is up to 30%higher than the existing DFSA standard scheme,and has more significant advantages,which is suitable for application in largescale RFID tags scenarios.
基金supported in part by the Joint Project of National Natural Science Foundation of China(U22B2004,62371106)in part by China Mobile Research Institute&X-NET(Project Number:2022H002)+6 种基金in part by the Pre-Research Project(31513070501)in part by National Key R&D Program(2018AAA0103203)in part by Guangdong Provincial Research and Development Plan in Key Areas(2019B010141001)in part by Sichuan Provincial Science and Technology Planning Program of China(2022YFG0230,2023YFG0040)in part by the Fundamental Enhancement Program Technology Area Fund(2021-JCJQ-JJ-0667)in part by the Joint Fund of ZF and Ministry of Education(8091B022126)in part by Innovation Ability Construction Project for Sichuan Provincial Engineering Research Center of Communication Technology for Intelligent IoT(2303-510109-04-03-318020).
文摘Addressing the challenges of passive Radio Frequency Identification(RFID)indoor localization technology in Non-Line-of-Sight(NLoS)and multipath environments,this paper presents an innovative approach by introducing a combined technology integrating an improved Kalman Filter with Space Domain Phase Difference of Arrival(SD-PDOA)and Received Signal Strength Indicator(RSSI).This methodology utilizes the distinct channel characteristics in multipath and NLoS contexts to effectively filter out interference and accurately extract localization information,thereby facilitating high precision and stability in passive RFID localization.The efficacy of this approach is demonstrated through detailed simulations and empirical tests conducted on a custom-built experimental platform consisting of passive RFID tags and an R420 reader.The findings are significant:in NLoS conditions,the four-antenna localization system achieved a notable localization accuracy of 0.25 m at a distance of 5 m.In complex multipath environments,this system achieved a localization accuracy of approximately 0.5 m at a distance of 5 m.When compared to conventional passive localization methods,our proposed solution exhibits a substantial improvement in indoor localization accuracy under NLoS and multipath conditions.This research provides a robust and effective technical solution for high-precision passive indoor localization in the Internet of Things(IoT)system,marking a significant advancement in the field.
基金supported by the Science and Technology Project of State Grid Jiangxi Electric Power Corporation Limited‘Research on Key Technologies for Non-Intrusive Load Identification for Typical Power Industry Users in Jiangxi Province’(521852220004)。
文摘Studying user electricity consumption behavior is crucial for understanding their power usage patterns.However,the traditional clustering methods fail to identify emerging types of electricity consumption behavior.To address this issue,this paper introduces a statistical analysis of clusters and evaluates the set of indicators for power usage patterns.The fuzzy C-means clustering algorithm is then used to analyze 6 months of electricity consumption data in 2017 from energy storage equipment,agricultural drainage irrigation,port shore power,and electric vehicles.Finally,the proposed method is validated through experiments,where the Davies-Bouldin index and profile coefficient are calculated and compared.Experiments showed that the optimal number of clusters is 4.This study demonstrates the potential of using a fuzzy C-means clustering algorithmin identifying emerging types of electricity consumption behavior,which can help power system operators and policymakers to make informed decisions and improve energy efficiency.
基金the National Natural Science Fund for Distinguished Young Scholars(22025803)supported by the National Natural Science Foundation of China(22178338)+1 种基金the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(YLU-DNL Fund 2021018)the financial support of project“Research and development and industrial application of new catalytic materials for green synthesis of MMA to replace highly toxic HCN”(Hebei,20374002D)。
文摘The kinetic behavior of esterification between methacrylic acid and methanol catalyzed by NKC-9 resin was studied in a fixed bed reactor.The reaction was conducted in the temperature range of 323.15 to 368.15 K with the molar ratio of reactants from 0.8 to 1.4 under certain pressure.The measurement data were regression with the pseudo-homogeneous(P-H),Eley-Rideal(E-R),and Langmuir-Hinshelwood(L-H)heterogeneous kinetic models.Independent adsorption experiments were implemented to gain the adsorption equilibrium constants of four components.Among the above three models,the L-H model exhibited the best fitting results.The stability of NKC-9 was evaluated by long-term running with the yield of methyl methacrylate no decrease during 3000 h operation.The structure and physicochemical properties of the new and used catalyst were performed by several characterizations including thermogravimetric analysis(TG),scanning electron microscope(SEM),X-ray diffraction(XRD)and Fourier transform infrared spectroscopy(FT-IR)and so on.
基金supported by the National Natural Science Foundation of China(Nos.22173075,21933012,31871877)the National Key Research and Development Program of China(2017YFA0204902)the Fundamental Research Funds for the Central Universities(Nos.20720200068,20720190002).
文摘Developments in advanced manufacturing have promoted the miniaturization of semiconductor electronic devices to a near-atomic scale,which continuously follows the‘top-down’construction method.However,huge challenges have been encountered with the exponentially increased cost and inevitably prominent quantum effects.Molecular electronics is a highly interdisciplinary subject that studies the quantum behavior of electrons tunneling in molecules.It aims to assemble electronic devices in a‘bottom-up’manner on this scale through a single molecule,thereby shedding light on the future design of logic circuits with new operating principles.The core technologies in this field are based on the rapid development of precise fabrication at a molecular scale,regulation at a quantum scale,and related applications of the basic electronic component of the‘electrode-molecule-electrode junction’.Therefore,the quantum charge transport properties of the molecule can be controlled to pave the way for the bottom-up construction of single-molecule devices.The review firstly focuses on the collection and classification of the construction methods for molecular junctions.Thereafter,various characterization and regulation methods for molecular junctions are discussed,followed by the properties based on tunneling theory at the quantum scale of the corresponding molecular electronic devices.Finally,a summary and perspective are given to discuss further challenges and opportunities for the future design of electronic devices.
文摘We report a rare case of intratumoral hemorrhage during postoperative radiotherapy for pituitary adenoma. A 57-year-old Asian male, complaining of long-standing eye strain, underwent a medical checkup of the brain. Magnetic resonance imaging showed a multicystic giant pituitary adenoma. The patient underwent an endoscopic endonasal transsphenoidal partial removal of the adenoma to provide optic pathway decompression and got relief from the visual symptoms. Just before completion of the postoperative radiotherapy for residual adenoma, the patient developed right hemiparesis, mild motor aphasia, and right oculomotor palsy. A cranial CT scan showed intratumoral hemorrhage into the intratumoral cyst. The patient therefore had to undergo three additional craniotomies for evacuation of cyst contents over the next 8 months. The follow-up MRI at 11 months after the initial hemorrhage showed that the new oozing of blood in the intratumoral cyst was still appearing. Intratumoral hemorrhage is a rare, albeit life-threatening, complication of pituitary adenoma. We reviewed relevant literature and suggested that the cystic component in pituitary adenoma could be a key pathogenesis of this rare complication. In conclusion, we suggest that it may be necessary to realize that cases which have cystic giant pituitary adenoma may cause hemorrhage by chance with the foreseeability.
基金supported by the National Natural Science Foundation of China(Nos.22250003,22173075,21933012,and 22003052)the Fundamental Research Funds for the Central Universities(Nos.20720220020,20720220072,and 20720200068).
文摘Metallic clusters,ranging from 1 to 2 nm in size,have emerged as promising candidates for creating nanoelectronic devices at the single-cluster level.With the intermediate quantum properties between metals and semiconductors,these metallic clusters offer an alternative pathway to silicon-based electronics and organic molecules for miniaturized electronics with dimensions below 5 nm.Significant progress has been made in studies of single-cluster electronic devices.However,a clear guide for selecting,synthesizing,and fabricating functional single-cluster electronic devices is still required.This review article provides a comprehensive overview of single-cluster electronic devices,including the mechanisms of electron transport,the fabrication of devices,and the regulations of electron transport properties.Furthermore,we discuss the challenges and future directions for single-cluster electronic devices and their potential applications.
基金supported by the National Natural Science Foundation of China(22325303,21973079,22032004)the National Key R&D Program of China(2017YFA0204902)+2 种基金the Fundamental Research Funds for the Central Universities in China(Xiamen University,20720190002)IRTSTFJ,National Science Foundation of Fujian Province(2018J06004)Beijing National Laboratory for Molecular Sciences(BNLMS202005).
文摘Charge transport characterization of single-molecule junctions is essential for the fundamental research of single-molecule physical chemistry and the development towards single-molecule electronic devices and circuits. Among the single-molecule conductance characterization techniques,the single-molecule break junction technique is widely used in tens of worldwide research laboratories which can generate a large amount of experimental data from thousands of individual measurement cycles. However,data interpretation is a challenging task for researchers with different research backgrounds,and the different data analysis approaches sometimes lead to the misunderstanding of the measurement data and even reproducibility issues of the measurement. It is thus a necessity to develop a user-friendly all-in-one data analysis tool that automatizes the basic data analysis in a standard and widely accepted way. In this work,we present the XMe Code (Xiamen Molecular Electronics Code),an intelligent all-in-one data analysis tool for the comprehensive analysis of single-molecule break junction data. XMe code provides end-to-end data analysis that takes in the original experimental data and returns electronic characteristics and even charge transport mechanisms. We believe that XMe Code will promote the transparency of the data analysis in single-molecule electronics and the collaborations among scientists with different research backgrounds.
基金National Natural Science Foundation of China(grant number 82088101 and 81930013 to Y.-H.C.,31871491 to J.Y.,82070338 and 82222008 to D.X.,82370396 to D.S.,82122007 to D.L.)National Key Research and Development Plan(grant number 2019YFA0801501 to Y.-H.C.)+4 种基金Program for the Research Unit of Origin and Regulation of Heart Rhythm,Chinese Academy of Medical Sciences(grant number 2019RU045 to Y.-H.C.)Top-Level Clinical Discipline Project of Shanghai Pudong(grant number PWYgf2021-01 to Y.-H.C.)Key Research Center Construction Project of Shanghai(grant number 2022ZZ01008 to Y.-H.C.)Shanghai Key Clinical Specialty Project(shslczdzk06202 to Y.-H.C.)National Key Clinical Specialty and Fundamental Research Funds for the Central Universities to Y.-H.C.
文摘Cardiac biological pacing(BP)is one of the future directions for bradyarrhythmias intervention.Currently,cardiac pacemaker cells(PCs)used for cardiac BP are mainly derived from pluripotent stem cells(PSCs).However,the production of high-quality cardiac PCs from PSCs remains a challenge.Here,we developed a cardiac PC differentiation strategy by adopting dual PC markers and simulating the developmental route of PCs.First,two PC markers,Shox2 and Hcn4,were selected to establish Shox2:EGFP;Hcn4:mCherry mouse PSC reporter line.Then,by stepwise guiding naïve PSCs to cardiac PCs following naïve to formative pluripotency transition and manipulating signaling pathways during cardiac PCs differentiation,we designed the FSK method that increased the yield of SHOX2^(+);HCN4^(+)cells with typical PC characteristics,which was 12 and 42 folds higher than that of the embryoid body(EB)and the monolayer M10 methods respectively.In addition,the in vitro cardiac PCs differentiation trajectory was mapped by single-cell RNA sequencing(scRNA-seq),which resembled in vivo PCs development,and ZFP503 was verified as a key regulator of cardiac PCs differentiation.These PSC-derived cardiac PCs have the potential to drive advances in cardiac BP technology,help with the understanding of PCs(patho)physiology,and benefit drug discovery for PC-related diseases as well.
基金supported by the National Natural Science Foundation of China(grant nos.22173075,21933012,61901402,31871877,and 21774106)the National Key R&D Program of China(grant no.2017YFA0204902)+1 种基金the Fundamental Research Funds for the Central Universities(grant nos.20720200068 and 20720190002)the Natural Science Foundation of Fujian Province(grant no.2018J06004).
文摘Spiropyran derivatives are prototype mechanophores with a promising application as molecular sensors because of their changeable structure under external force stimuli.However,the chemical structure evolution under external stimuli remains unclear due to the uncertainty and difficulty in distinguishing the structures of different ring-opened merocyanine isomers generated in the force-induced reaction.Here we identify the structure of isomers produced by the force-induced reaction of spiropyran derivatives using a single-molecule conductance measurement and an unsupervised clustering algorithm.We found that the original data from the single-molecule conductance measurement can be divided into four clusters through unsupervised clustering.By introducing a photoinduced reaction and theoretical calculation,we identified and attributed the four clusters of data to the multiple states of the molecular junctions.Our work demonstrates that a single-molecule break junction measurement can distinguish the isomers in the force-induced reaction,suggesting the great potential of single-molecule conductance measurement and unsupervised clustering approaches for structural analysis.
基金supported by the National Natural Science Foundation of China(21722305,21933012,31871877)the National Key R&D Program of China(2017YFA0204902)+4 种基金Natural Science Foundation of Fujian Province(2018J06004)Beijing National Laboratory for Molecular Sciences(BNLMS202010 and BNLMS202005)the Fundamental Research Funds for the Central Universities(20720220020,20720220072,20720200068,20720190002)supported by the Engineering and Physical Sciences Research Council(EPSRC,EP/M014452/1,EP/P027156/1,and EP/N03337X/1)the European Commission,the Future and Emerging Technologies(FET)Open project 767187-QuIET and the European(EU)project Bac-to-Fuel.
文摘Sorting out organic molecules with high thermopower is essential for understanding molecular thermoelectrics.The intermolecular coupling offers a unique chance to enhance the thermopower by tuning the bandgap structure of molecular devices,but the investigation of intermolecular coupling in bulk materials remains challenging.Herein,we investigated the thermopower of diketopyrrolopyrrole(DPP)cored single-molecule junctions with different coupling strengths by varying the packing density of the self-assembled monolayers(SAM)using a customized scanning tunneling microscope break junction(STM-BJ)technique.We found that the thermopower of DPP molecules could be enhanced up to one order of magnitude with increasing packing density,suggesting that the thermopower increases with larger neighboring intermolecular interactions.The combined density functional theory(DFT)calculations revealed that the closely-packed configuration brings stronger intermolecular coupling and then reduces the highest occupied molecular orbital(HOMO)-lowest unoccupied molecular orbital(LUMO)gap,leading to an enhanced thermopower.Our findings offer a new strategy for developing organic thermoelectric devices with high thermopower.
基金J.Liu acknowledges the support of the Guangdong Basic and Applied Basic Research Foundation(No.2021A1515010188)the Shenzhen Science and Technology Innovation Committee(No.JCYJ20190809181011411)+1 种基金the Guangdong Department of Education(No.2021ZDJS097)Y.Xie gratefully acknowledges the financial support from the National Natural Science Foundation of China(No.22107058).
文摘Many cyclobutane natural products have intriguing biological properties that arise from their fascinating chemical structures.Cyclobutane natural products feature a cyclobutane scaffold as the core or as a part of the spirocyclic or fused cyclic core.However,the highly functionalized nature and the inherent stereochemistry of these cyclobutane natural products,which are associated with their biological activities,pose tremendous challenges to their preparation.In this perspective,we present contemporary advancements in synthetic methods and/or strategies en route to the bioactive cyclobutane natural products.We begin by describing the representative bioactive cyclobutane natural products and then focus on illustrative examples of their syntheses reported from 2018 to 2021.These advances will enable efficient syntheses of cyclobutanes of structural and biological importance.
文摘We report an electrochemically assisted mechanically controllable break junction (EC-MCBJ) approach to investigating single molecule conductance. Electrode pairs connected with a gold nanobridge were fabricated by electrochemical deposition and then mounted on a homebuilt MCBJ platform. A large number of Au- molecule-Au junctions were produced sequentially by repeated breaking and reconnecting of the gold nanobridge. In order to measure their single molecule conductance, statistical conductance histograms were generated for benzene-l,4-dithiol (BDT) and 4,4'-bipyridine (BPY). The values extracted from these histograms were found to be in the same range as values previously reported in the literature. Our method is distinct from the ones used to acquire these previously reported literature values, however, in that it is faster, simpler, more cost-effective, and changing the electrode material is more convenient.
基金supported by the National Key R&D Program of China (2017YFA0204901, 2017YFA0204902)the National Natural Science Foundation of China (21673195, 61571242, 21503179, 21727806, 21722305)the Young Thousand Talent Project of China
文摘Benefiting from the development of molecular electronics and molecular plasmonics, the interplay of light and electronic transport in molecular junctions has attracted growing interest among researchers in both fields, leading to a new research direction of "single-molecule optoelectronics". Here, we review the latest developments of photo-modulated charge transport,electroluminescence and Raman spectroscopy from single-molecule junctions, and suggest future directions for single-molecule optoelectronics.
基金Acknowledgements This work was supported by the National Natural Science Foundation of China (Nos. 21503179, 21403181, 61573295, 21522508, 21673195, 21533006, and 61071010), the National Basic Research Program of China (No. 2015CB932300), the Natural Science Foundation of Fujian Province (No. 2016J05162), the Fundamental Research Funds for the Central Universities in China (Xiamen University, Nos. 20720170035 and 20720160092), and the Young Thousand Talent Project of China.
文摘In this article, we report on the fabrication and transport measurements of Cu quantum point contacts prepared by a novel, electrochemically assisted mechanically controllable break junction (EC-MCBJ) method. By employing photolithography and wet-etching processes, suspended electrode pairs were patterned and fabricated successfully on Si microchips. Rather than adopting an acid Cu electroplating solution, a novel alkaline electroplating solution was developed and utilized to establish Cu nanocontacts between electrode pairs. Typically, the widths of the as-fabricated Cu nanocontacts were found to be smaller than 18 nm. A large number of Cu quantum point contacts were then produced and characterized by a home-built MCBJ setup. In addition to the conventional histogram, where peaks tend to decrease in amplitude with increasing conductance, an anomalous type of conductance histogram, exhibiting different peak amplitudes, was observed. Through statistical analysis of the maximum allowable bending of the Si microchips, and theoretical calculations, we demonstrated that our alkaline Cu electroplating solution affords Cu nanocontacts that are compatible with subsequent MCBJ operations, which is essential for the fabrication of Cu quantum point contacts. As sophisticated e-beam lithography is not required, the EC-MCBJ method is fast, simple, and cost-effective. Moreover, it is likely to be suitable for the fabrication and characterization of quantum point contacts of various metals from their respective electroplating solutions.
基金This work was supported by the National Basic Research Program of China (Nos. 2011YQ030124, 2014CB845603, and 2015CB932301), National Natural Science Foundation of China (Nos. 91427304, 21321062, 21303114, 21403181, and 21503179), Natural Science Foundation of Fujian Province (No. 2012J05034), and by CNRS UMR 8640 PASTEUR and LIA CNRS NanoBioCatEchem.
文摘In this article, we report on the characterization of various molecular junctions' current-voltage characteristics (Ⅰ-Ⅴ curves) evolution under mechanical modulations, by employing a novel electrochemically assisted-mechanically controllable break junction (EC-MCBJ) method. For 1,4-benzenedithiol, the Ⅰ-Ⅴ curves measured at constant electrode pair separation show excellent reproducibility, indicating the feasibility of our EC-MCBJ method for fabricating molecular junctions. For ferrocene-bisvinylphenylmethyl dithiol (Fc-VPM), an anomalous type of Ⅰ-Ⅴ curve was observed by the particular control over the stepping motor. This phenomenon is rationalized assuming a model of atomic contact evolution with the presence of molecular junctions. To test this hypothesized model, a molecule with a longer length, 1,3-butadiyne-linked dinuclear ruthenium(H) complex (Ru-1), was implemented, and the Ⅰ-Ⅴ curve evolution was investigated under similar circumstances. Compared with Fc-VPM, the observed Ⅰ-Ⅴ curves show close analogy and minor differences, and both of them fit the hypothesized model well.
基金This work was supported by the National Natural Science Foundation of China(21673195,21722305,21703188,U1705254,21933012,31871877)the National Key R&D Program of China(2017YFA0204902),the Fundamental Research Funds for the Central Universities(20720200068)the Fundamental Research Funds for Xiamen University(20720190002).
文摘Molecular rectifier, as a basic function of molecular electronic devices, has attracted extensive attention for the opportunity in constructing sub-nanometer electronic devices. However, tunneling leakage current has a significant contribution as electronic devices shrink in size, which leads to a challenge in fabricating molecular rectifiers at the sub-nanometer scale. Here, we experimentally demonstrate a sub-nanometer molecular rectifier based on the supramolecular junction assembled between water and 1,4-diazabicyclo[2.2.2]octane (DABCO) molecule. The charge transport through DABCO and corresponding supramolecular junctions exhibits destructive σ-interference, ensuring a sharp conductance variation for transmission modulation. The supramolecular interaction between DABCO and water readily introduces the asymmetric electrode-molecule interaction, which combines with the destructive σ-interference to support the sub-nanometer rectification.
基金supported by the National Key R&D Project of China(2017YFA0204902)the National Natural Science Foundation of China(21722305,21673195,21703188,21790360)the Youth Innovation Promotion Association CAS(2015024)
文摘The conductance through single-molecule junctions characterized by the break junction techniques consists of the through-space tunneling and through-molecule tunneling conductance, and the existence of through-space tunneling between the electrodes makes the quantitative extraction of the intrinsic molecular signals of single-molecule junctions challenging. Here, we established an analytic model to describe the evolution of the conductance of a single molecule in break junction measurements. The experimental data for a series of oligo(aryleneethynylene) derivatives validate the proposed model, which provides a modeling insight into the conductance evolution for the opening process in a "real" break junction experiment. Further modulations revealed that the junction formation probability and rupture distance of the molecular junction, which reflect the junction stability, will significantly influence the amplitude and position of the obtained conductance peak. We further extend our model to a diffusion and a chemical reaction process, for which the simulation results show that the break junction technique offers a quantitative understanding of these time-dependent systems, suggesting the potential of break junction techniques in the quantitative characterization of physical and chemical processes at the single-molecule scale.
基金supported by the National Natural ScienceFoundation of China (Nos. 22173075, 21933012 and 31871877)the National Key R&D Program of China (No. 2017YFA0204902)+1 种基金the Fundamental Research Funds for the Central Universities(Nos. 20720200068 and 20720190002)the Beijing NationalLaboratory for Molecular Sciences (No. BNLMS202005).
文摘The investigation of electronic excited states in single-molecule junctions not only provides platforms to reveal the photophysical and photochemical processes at the molecular level,but also brings opportunities for the development of single-molecule optoelectronic devices.Understanding the interaction mechanisms between molecules and nanocavities is essential to obtain ondemand properties in devices by artificial design,since molecules in junctions exhibit unique behaviors of excited states benefited from the structures of metallic nanocavities.Here,we review the excitation mechanisms involved in the interplay between molecules and plasmonic nanocavities,and reveal the influence of nanostructures on excited-state properties by demonstrating the differences in excited state decay processes.Furthermore,vibronic transitions of molecules between nanoelectrodes are also discussed,offering a new single-molecule characterization method.Finally,we provide the potential applications and challenges in single-molecule optoelectronic devices and the possible directions in exploring the underlying mechanisms of photophysical and photochemical processes.
基金supported by the Ministry of Science and Technology of China(No. SQ2017YFJC020081)the National Natural Science Foundation of China(Nos. 21673195,21503179)+2 种基金Fundamental Research Funds for the Central Universities in China (Xiamen University: No. 20720170035)Natural Science Foundation of Fujian Province(No. 2016J05162)the Young Thousand Talent Project of China
文摘The quantum interference effect in the charge transport through single-phenyl molecules received intensive interests from theory but remained as an experimental challenge. In this paper, we investigated the charge transport through single-molecule benzene dithiol (BDT) junction with different connectivities using mechanically controllable break.junction (MCB]) technique. By further improving the mechanical stability and the electronic measuring component of the MCBJ set-up, we obtained the conductance histograms of BDT molecules (BDTs) from the statistical analysis of conductance-distance traces without data selection. By tuning the connectivity, the conductance of BDTs is determined to be 10-12Go, 10-22Go and 10-10Go for pcra, meta, and ortho connectivity, following the trend that ortfio-BDT 〉 para-BDT 〉 meta-BDT. Furthermore, the displacements of the junctions followed the trend that para 〉 meta 〉 ortho, suggesting the charge transport through the molecules via the gold-thiol bond. The different trends between conductance and displacement for different connectivities suggests the presence of destructive quantum interference effect on meta-BDT, which provides the experimental evidence for the quantum interference effect through single-phenyl molecular junctions.