A precise theoretical investigation has been made on the cylindrical and spherical (nonplanar) Gardner solitons (GSs) and double layers (DLs) in a dusty electronegative plasma (composed of inertial positive and...A precise theoretical investigation has been made on the cylindrical and spherical (nonplanar) Gardner solitons (GSs) and double layers (DLs) in a dusty electronegative plasma (composed of inertial positive and negative ions, Maxwellian cold electrons, non-thermal hot electrons, and negatively charged static dust). The reductive perturbation method has been used in derivation of the modified Gardner (MG) equation describing the nonlinear propagation of the dust ion-acoustic (DIA) waves. The MG equation admits solitary waves (SWs) and DLs solutions for σ around its critical value σ c (where σc is the value of σ corresponding to the vanishing of the nonlinear coefficient of the Korteweg de-Vries (K-dV) equation). The nonplanar SWs and DLs solutions are numerically analyzed and the parametric regimes for the existence of the positive as well as negative SWs and negative DLs are obtained. The basic features of nonplanar DIA SWs and DLs, which are found to be different from planar ones, are also identified. The implications of our results to different space and laboratory dusty plasma situations, are discussed.展开更多
We consider a steady-state(but transient)situation in which a warm dense aggregate is a two-temperature system with equilibrium electrons at temperature T_(e),ions at T_(i),and T_(e)≠T_(i).Such states are achievable ...We consider a steady-state(but transient)situation in which a warm dense aggregate is a two-temperature system with equilibrium electrons at temperature T_(e),ions at T_(i),and T_(e)≠T_(i).Such states are achievable by pump–probe experiments.For warm dense hydrogen in such a twotemperature situation,we investigate nuclear quantum effects(NQEs)on structure and thermodynamic properties,thereby delineating the limitations of ordinary ab initio molecular dynamics.We use path integral molecular dynamics(PIMD)simulations driven by orbital-free density functional theory(OFDFT)calculations with state-of-the-art noninteracting free-energy and exchange-correlation functionals for the explicit temperature dependence.We calibrate the OFDFT calculations against conventional(explicit orbitals)Kohn–Sham DFT.We find that when the ratio of the ionic thermal de Broglie wavelength to the mean interionic distance is larger than about 0.30,the ionic radial distribution function is meaningfully affected by the inclusion of NQEs.Moreover,NQEs induce a substantial increase in both the ionic and electronic pressures.This confirms the importance of NQEs for highly accurate equation-of-state data on highly driven hydrogen.For Te>20 kK,increasing Te in the warm dense hydrogen has slight effects on the ionic radial distribution function and equation of state in the range of densities considered.In addition,we confirm that compared with thermostatted ring-polymer molecular dynamics,the primitive PIMD algorithm overestimates electronic pressures,a consequence of the overly localized ionic description from the primitive scheme.展开更多
The triple bond in N_(2)has an extremely high bond energy and is thus difficult to break.N_(2)is commonly converted into NH3 artificially via the Haber-Bosch process,and NH_(3)can be utilized to produce other nitrogen...The triple bond in N_(2)has an extremely high bond energy and is thus difficult to break.N_(2)is commonly converted into NH3 artificially via the Haber-Bosch process,and NH_(3)can be utilized to produce other nitrogen-containing chemicals.Here,we developed an electron catalyzed method to directly fix N_(2)into azos,by pushing and pulling the electron into and from the aromatic halide with the cyclic voltammetry method.The round-trip journey of electron can successfully weaken the triple bond in N_(2)through the electron pushing-induced aryl radical via a“brick trowel”transition state,and then produce the diazonium ions by pulling the electron out from the diazo radical intermediate.Different azos can be synthesized with this developed electron catalyzed approach.This approach provides a novel concept and practical route for the fixation of N_(2)at atmospheric pressure into chemical products valuable for industrial and commercial applications.展开更多
The features of optical defects in a chemical vapor deposition (CVD) synthetic type Ⅱ a diamond were characterized using photoluminescence (PL) spectroscopy, before and after electron irradiation. The sample was cut ...The features of optical defects in a chemical vapor deposition (CVD) synthetic type Ⅱ a diamond were characterized using photoluminescence (PL) spectroscopy, before and after electron irradiation. The sample was cut within a {100} growth layer, and irradiated with 2 MeV electrons along the <100> axis. PL spectra of sample were collected under 532 nm and 355 nm laser excitation, at room temperature and 77 K, and linear scanning analysis along incident depth was applied to determine the distribution of defects. The pre-irradiation characterization results revealed uniformly distributed PL centers at 389 nm, 469 nm, 533 nm, 575 nm (ZPL of NV 0), 637 nm (ZPL of NV -), and 736.7/737.1 nm (ZPL doublet of SiV -). After irradiation, the differential responses of these as-grown defects were observed, alongside the emergence of irradiation-induced defects, namely 489 nm center, H3 center (ZPL at 504 nm) and GR1 center (ZPL at 741 nm). The maximum penetration depth of 2 MeV electron-irradiation induced defects was determined to be 2.1 mm. This work primarily presents the depth profiles of both as-grown and irradiation-induced defects in 2 MeV electrons irradiated diamond. The result provides experimental data for better understanding of the radiation effect in diamonds. Serving as a reference for diamond enhancement by electron irradiation.展开更多
The gold nano-plates(Au NPLs)have been extensively studied for their high quality factor as mechanical resonators.But it remains still unclear how the thickness and morphology of Au NPLs affect the hot electron diffus...The gold nano-plates(Au NPLs)have been extensively studied for their high quality factor as mechanical resonators.But it remains still unclear how the thickness and morphology of Au NPLs affect the hot electron diffusion.Here we have employed transient absorption microscopy to gain spatiotemporal imaging of the hot electron diffusion in Au NPLs.Au NPLs of varying thickness over 200 nm were synthesized.It was found that the hot electron diffusion of Au NPL excited at the boundary is obviously faster than that excited at the internal surface.And thinner Au NPLs exhibit a faster hot electron diffusion rate compared to thicker Au NPLs.Because the time constant of hot electron cooling(electron-phonon coupling)is independent of the excited position and thickness of Au NPLs,the effect of electron-phonon coupling on hot electron diffusion should be ruled out.So the hot electron diffusion rate is highly dimensionality-dependent.The quasi-one-dimensional diffusion along the boundary of nanoplate has the fastest rate of 50 cm^(2)/s,and the three-dimensional diffusion has the slowest rate of 22 cm^(2)/s.The fundamental investigation on the hot electrons transport property of Au NPLs offers a new insight for designing metal-based optoelectronic devices.展开更多
The propagation properties of ion-acoustic solitary and shock waves in the magnetized viscous plasma with nonthermal trapped electrons are investigated.The Cairns-Gurevich distribution as the electron distribution is ...The propagation properties of ion-acoustic solitary and shock waves in the magnetized viscous plasma with nonthermal trapped electrons are investigated.The Cairns-Gurevich distribution as the electron distribution is considered to describe the plasma nonthermality and particle trapping.By adopting the reductive perturbation technique,we derived the nonlinear Schamel-Korteweg-de Vries-Burgers(SKdVB)equation,and then obtained the ion-acoustic shock and solitary wave solutions of the SKdVB equation for different limiting cases.It is found that the impact of nonthermal parameterα,external magnetic fieldΩ,obliqueness lz,wave speed U0,and the ion kinematic viscosityη0can significantly change the characteristics of the shock and solitary waves.These results may be useful for better understanding the propagation of nonlinear structures in space(i.e.Earth's magnetosphere and ionosphere,auroral regions)and laboratory plasma with nonthermal trapped electrons.展开更多
The susceptibility of Pt catalyst surfaces to carbon monoxide(CO)poisoning in anodic hydrogen oxidation reaction(HOR)has been a critical constraint on the development of proton exchange membrane fuel cells(PEMFCs).Eff...The susceptibility of Pt catalyst surfaces to carbon monoxide(CO)poisoning in anodic hydrogen oxidation reaction(HOR)has been a critical constraint on the development of proton exchange membrane fuel cells(PEMFCs).Effectively regulating the electronic structure of Pt to enhance CO resistance is crucial for developing high-performance catalysts with robust anti-poisoning capabilities.Herein,the Pt/W@NCNF featured by Pt nanoparticles and atomical dispersed tungsten(W)sites on N-doped carbon nanofibers is developed for CO tolerance HOR catalyst.The presence of W enables the electron transfer from Pt,which promotes electron rearrangement in the Pt-5d orbitals.It not only optimizes the adsorption of H^(*) and CO^(*)on Pt,but also the OH^(*) intermediates adsorbed on the W sites oxidize the CO*adsorbed on Pt,thereby retaining more active sites for H_(2) adsorption and oxidation.The HOR exchange current density of Pt/W@NCNF reaches 1.35 times that of commercial Pt/C,and the limiting current density decreases by only 3.4%after introducing 1000 ppm CO in H_(2).Notably,the Pt/W@NCNF-based PEMFCs deliver markedly superior performance across a range of CO concentrations.The present study demonstrates that electronic modulation of Pt is an effective strategy for simultaneously achieving resistance to CO and promoted HOR activity.展开更多
Stretchable electronics have been recognized as intriguing next-generation electronics that possess huge market value,and stretchable electronic conductors(SECs)are essential for stretchable electronics,which not only...Stretchable electronics have been recognized as intriguing next-generation electronics that possess huge market value,and stretchable electronic conductors(SECs)are essential for stretchable electronics,which not only can serve as critical functional components but also are the indispensable electronic connections bridging various electronic components within stretchable electronic systems.Herein,we offer a comprehensive review of recent progress in SECs including the material categories,structure designs,fabrication techniques,and applications.The characteristics,performance enhancement strategies,and application requirements are emphasized.Based on the recent advances,the existing challenges and future prospects are outlined and discussed.展开更多
Permeable electronics promise improved physiological comfort,but remain constrained by limited functional integration and poor mechanical robustness.Here,we report a three-dimensional(3D)permeable electronic system th...Permeable electronics promise improved physiological comfort,but remain constrained by limited functional integration and poor mechanical robustness.Here,we report a three-dimensional(3D)permeable electronic system that overcomes these challenges by combining electrospun SEBS nanofiber mats,high-resolution liquid metal conductors patterned via thermal imprinting(50μm),and a strain isolators(SIL)that protects vertical interconnects(VIAs)from stress concentration.This architecture achieves ultrahigh air permeability(>5.09 m L cm^(-2)min^(-1)),exceptional stretchability(750%fracture strain),and reliable conductivity maintained through more than 32,500 strain cycles.Leveraging these advances,we have integrated multilayer circuits,strain sensors,and a three-axis accelerometer to achieve a fully integrated,stretchable,permeable wireless real-time gesture recognition glove.The system enables accurate sign language interpretation(98%)and seamless robotic hand control,demonstrating its potential for assistive technologies.By uniting comfort,durability,and high-density integration,this work establishes a versatile platform for nextgeneration wearable electronics and interactive human-robot interfaces.展开更多
The effects of initial spin orientation on the final electron beam polarization in laser wakefield acceleration in a pre-polarized plasma are investigated theoretically and numerically.From the results of variation of...The effects of initial spin orientation on the final electron beam polarization in laser wakefield acceleration in a pre-polarized plasma are investigated theoretically and numerically.From the results of variation of the initial spin direction,the spin dynamics of the electron beam are found to depend on the self-injection mechanism.The effects of wakefields and laser fields are studied using test particle dynamics and particle-in-cell simulations based on the Thomas-Bargmann-Michel-Telegdi equation.Compared with transverse injection,longitudinal injection is found to be preferable for obtaining a highly polarized electron beam.展开更多
The discovery of pressure-induced superconducting electrides has sparked a intense wave of interest in novel superconductors.However,opinions vary regarding the relationship between non-nuclear attractors(NNAs)and sup...The discovery of pressure-induced superconducting electrides has sparked a intense wave of interest in novel superconductors.However,opinions vary regarding the relationship between non-nuclear attractors(NNAs)and superconductivity,with two opposing views currently represented by the materials Li_(6)P and Li_(6)C.Here,we choose the ternary Li–C–P as a model system and reveal the underlying mechanism by which NNAs contribute to superconductivity.The loosely bound NNAs in the superlithide Li_(14)CP covalently bond with Li and form unique satellite interstitial electrons(SIEs)around Li near the Fermi level,dominating the superconductivity.First-principles calculations show that the SIEs progressively increase in number and couple strongly with phonons at high pressure.Moreover,the Fermi surface nesting associated with SIEs induces phonon softening,further enhancing the electron–phonon coupling and giving the superlithide Li_(14)CP a T_(c)of 10.6 K at 300 GPa.The leading role of SIEs in superconductivity is a general one and is also relevant to the recently predicted Li_(6)P and Li_(6)C.Our work presented here reshapes the understanding of NNA-dominated superconductivity and holds promise for guiding future discoveries and designs of novel high-temperature superconductors.展开更多
The rapid advancement of machine learning based tight-binding Hamiltonian(MLTB)methods has opened new avenues for efficient and accurate electronic structure simulations,particularly in large-scale systems and long-ti...The rapid advancement of machine learning based tight-binding Hamiltonian(MLTB)methods has opened new avenues for efficient and accurate electronic structure simulations,particularly in large-scale systems and long-time scenarios.This review begins with a concise overview of traditional tight-binding(TB)models,including both(semi-)empirical and first-principles approaches,establishing the foundation for understanding MLTB developments.We then present a systematic classification of existing MLTB methodologies,grouped into two major categories:direct prediction of TB Hamiltonian elements and inference of empirical parameters.A comparative analysis with other ML-based electronic structure models is also provided,highlighting the advancement of MLTB approaches.Finally,we explore the emerging MLTB application ecosystem,highlighting how the integration of MLTB models with a diverse suite of post-processing tools from linear-scaling solvers to quantum transport frameworks and molecular dynamics interfaces is essential for tackling complex scientific problems across different domains.The continued advancement of this integrated paradigm promises to accelerate materials discovery and open new frontiers in the predictive simulation of complex quantum phenomena.展开更多
Traditional digitizers for signal readout of PET detectors are based on commercial analog-to-digital converters(ADC).However,the cost and power consumption of an entire electronic readout system based on digitizers fo...Traditional digitizers for signal readout of PET detectors are based on commercial analog-to-digital converters(ADC).However,the cost and power consumption of an entire electronic readout system based on digitizers for a PET scanner are high.To address this problem,a soft-core ADC based on a field-programmable gate array(FPGA)was proposed.An FPGA-based ADC(FPGA-ADC)combines low loss and high performance.To achieve good performance,the FPGA-ADC requires three calibrations:time-to-digital converter(TDC)length calibration,TDC alignment calibration,and TDC-to-ADC calibration.A prototype front-end electronics based on FPGA-ADC was built to evaluate the performance of time-of-flight positron emission tomography(TOF PET)detectors.Each PET detector consists of a LYSO crystal single-ended coupled to a silicon photomultiplier(SiPM).The experimental results show that the full-width at half-maximum(FWHM)energy resolution for 511 keV gamma photons after saturation correction of the SiPM was 12.3%.The FWHM coincidence timing resolution(CTR)of the TOF PET detector with the readout of the front-end electronic prototype is 385.2 ps.FPGA-ADCbased front-end electronics are very promising for multichannel,low-cost,highly integrated,and power-efficient readout electronic systems for radiation detector applications.展开更多
A rapidly growing field is piezoresistive sensor for accurate respiration rate monitoring to suppress the worldwide respiratory illness.However,a large neglected issue is the sensing durability and accuracy without in...A rapidly growing field is piezoresistive sensor for accurate respiration rate monitoring to suppress the worldwide respiratory illness.However,a large neglected issue is the sensing durability and accuracy without interference since the expiratory pressure always coupled with external humidity and temperature variations,as well as mechanical motion artifacts.Herein,a robust and biodegradable piezoresistive sensor is reported that consists of heterogeneous MXene/cellulose-gelation sensing layer and Ag-based interdigital electrode,featuring customizable cylindrical interface arrangement and compact hierarchical laminated architecture for collectively regulating the piezoresistive response and mechanical robustness,thereby realizing the long-term breath-induced pressure detection.Notably,molecular dynamics simulations reveal the frequent angle inversion and reorientation of MXene/cellulose in vacuum filtration,driven by shear forces and interfacial interactions,which facilitate the establishment of hydrogen bonds and optimize the architecture design in sensing layer.The resultant sensor delivers unprecedented collection features of superior stability for off-axis deformation(0-120°,~2.8×10^(-3) A)and sensing accuracy without crosstalk(humidity 50%-100%and temperature 30-80).Besides,the sensor-embedded mask together with machine learning models is achieved to train and classify the respiration status for volunteers with different ages(average prediction accuracy~90%).It is envisioned that the customizable architecture design and sensor paradigm will shed light on the advanced stability of sustainable electronics and pave the way for the commercial application in respiratory monitory.展开更多
Electron beam injectors are pivotal components of large-scale scientific instruments,such as synchrotron radiation sources,free-electron lasers,and electron-positron colliders.The quality of the electron beam produced...Electron beam injectors are pivotal components of large-scale scientific instruments,such as synchrotron radiation sources,free-electron lasers,and electron-positron colliders.The quality of the electron beam produced by the injector critically influences the performance of the entire accelerator-based scientific research apparatus.The injectors of such facilities usually use photocathode and thermionic-cathode electron guns.Although the photocathode injector can produce electron beams of excellent quality,its associated laser system is massive and intricate.The thermionic-cathode electron gun,especially the gridded electron gun injector,has a simple structure capable of generating numerous electron beams.However,its emittance is typically high.In this study,methods to reduce beam emittance are explored through a comprehensive analysis of various grid structures and preliminary design results,examining the evolution of beam phase space at different grid positions.An optimization method for reducing the emittance of a gridded thermionic-cathode electron gun is proposed through theoretical derivation,electromagnetic-field simulation,and beam-dynamics simulation.A 50%reduction in emittance was achieved for a 50 keV,1.7 A electron gun,laying the foundation for the subsequent design of a high-current,low-emittance injector.展开更多
Achieving high-energy density remains a key objective for advanced energy storage systems.However,challenges,such as poor cathode conductivity,anode dendrite formation,polysulfide shuttling,and electrolyte degradation...Achieving high-energy density remains a key objective for advanced energy storage systems.However,challenges,such as poor cathode conductivity,anode dendrite formation,polysulfide shuttling,and electrolyte degradation,continue to limit performance and stability.Molecular and ionic dipole interactions have emerged as an effective strategy to address these issues by regulating ionic transport,modulating solvation structures,optimizing interfacial chemistry,and enhancing charge transfer kinetics.These interactions also stabilize electrode interfaces,suppress side reactions,and mitigate anode corrosion,collectively improving the durability of high-energy batteries.A deeper understanding of these mechanisms is essential to guide the design of next-generation battery materials.Herein,this review summarizes the development,classification,and advantages of dipole interactions in high-energy batteries.The roles of dipoles,including facilitating ion transport,controlling solvation dynamics,stabilizing the electric double layer,optimizing solid electrolyte interphase and cathode–electrolyte interface layers,and inhibiting parasitic reactions—are comprehensively discussed.Finally,perspectives on future research directions are proposed to advance dipole-enabled strategies for high-performance energy storage.This review aims to provide insights into the rational design of dipole-interactive systems and promote the progress of electrochemical energy storage technologies.展开更多
In this study,the dosimetric characteristics(thickness applicability,preheating time,temperature and humidity dependence,in-batch uniformity,readout reproducibility,dose linearity,self-decay,and electron energy respon...In this study,the dosimetric characteristics(thickness applicability,preheating time,temperature and humidity dependence,in-batch uniformity,readout reproducibility,dose linearity,self-decay,and electron energy response)of engineered polycarbonate films irradiated with an electron beam(0–600 kGy)were investigated using photoluminescence spectroscopy.The results show a linear relationship between photoluminescence intensity and radiation dose when the thickness of the polycarbonate film is 0.3 mm.A higher fluorescence intensity can be obtained by preheating at 60℃ for 180 min before photoluminescence spectrum analysis.As the temperature during spectral testing and the ambient humidity(during and after irradiation)increased,the photoluminescence intensity of the polycarbonate films decreased.The photoluminescence intensity deviation of the polycarbonate films produced within the same batch at 100 kGy is 2.73%.After ten times of repeated excitations and readouts,the coefficients of variation in photoluminescence intensity are less than 8.6%,and the linear correlation coefficient between photoluminescence intensity and irradiation dose is 0.965 in the dose capture range of 20–600 kGy.Within 60 days of irradiation,the photoluminescence intensity of the polycarbonate film decreased to 60%of the initial value.The response of the 0.3 mm polycarbonate films to electron beams with energies exceeding 3.5 MeV does not differ significantly.This comprehensive analysis indicates the potential of polycarbonate films as a high-radiation dose detection material.展开更多
We report a theoretical investigation into superconductivity within the MAXH_(6) quaternary hydride system using first-principles calculations,where M and A denote alkali and alkaline earth elements,respectively,and X...We report a theoretical investigation into superconductivity within the MAXH_(6) quaternary hydride system using first-principles calculations,where M and A denote alkali and alkaline earth elements,respectively,and X represents transition metal elements.Systematic analysis of electronic band structures,phonon dispersions,and electron-phonon coupling reveals that substitution of MA binary metal combinations and X metal atoms can create favorable conditions for superconductivity.Mapping of superconducting critical temperatures,combined with dynamical stability analysis through phonon calculations,identifies ten superconducting candidates at ambient pressure.Among these,LiNaAgH_(6) exhibits nearly-free-electron behavior reminiscent of monovalent electron superconductors.It demonstrates exceptional superconducting properties with electron–phonon coupling λ=2.707,which yields a superconducting transition temperature T_(c) of 206.4 K using the Allen–Dynes formula.Its structural analogs MgNaPdH_(6),LiMgPdH_(6),LiMgAgH_(6),LiMgAuH_(6) all exhibit superconducting transition temperatures above 110 K.These findings advance our fundamental understanding of superconductivity in quaternary hydrides and provide guidance for rational design of new high-temperature superconducting materials.展开更多
文摘A precise theoretical investigation has been made on the cylindrical and spherical (nonplanar) Gardner solitons (GSs) and double layers (DLs) in a dusty electronegative plasma (composed of inertial positive and negative ions, Maxwellian cold electrons, non-thermal hot electrons, and negatively charged static dust). The reductive perturbation method has been used in derivation of the modified Gardner (MG) equation describing the nonlinear propagation of the dust ion-acoustic (DIA) waves. The MG equation admits solitary waves (SWs) and DLs solutions for σ around its critical value σ c (where σc is the value of σ corresponding to the vanishing of the nonlinear coefficient of the Korteweg de-Vries (K-dV) equation). The nonplanar SWs and DLs solutions are numerically analyzed and the parametric regimes for the existence of the positive as well as negative SWs and negative DLs are obtained. The basic features of nonplanar DIA SWs and DLs, which are found to be different from planar ones, are also identified. The implications of our results to different space and laboratory dusty plasma situations, are discussed.
基金The majority of this work was done while D.K.was a visitor at the University of Florida.He was supported by the Science Challenge Project of China under Grant No.TZ2016001the NSFC under Grant No.11874424+3 种基金the National Key R&D Program of China under Grant No.2017YFA0403200He also acknowledges support by the China Scholarship Council.K.L.(for the majority of the work done while at the University of Florida)S.B.T.were supported by U.S.Department of Energy Grant No.DE-SC0002139Most of the computations were performed on the HiPerGator-II system at the University of Florida.
文摘We consider a steady-state(but transient)situation in which a warm dense aggregate is a two-temperature system with equilibrium electrons at temperature T_(e),ions at T_(i),and T_(e)≠T_(i).Such states are achievable by pump–probe experiments.For warm dense hydrogen in such a twotemperature situation,we investigate nuclear quantum effects(NQEs)on structure and thermodynamic properties,thereby delineating the limitations of ordinary ab initio molecular dynamics.We use path integral molecular dynamics(PIMD)simulations driven by orbital-free density functional theory(OFDFT)calculations with state-of-the-art noninteracting free-energy and exchange-correlation functionals for the explicit temperature dependence.We calibrate the OFDFT calculations against conventional(explicit orbitals)Kohn–Sham DFT.We find that when the ratio of the ionic thermal de Broglie wavelength to the mean interionic distance is larger than about 0.30,the ionic radial distribution function is meaningfully affected by the inclusion of NQEs.Moreover,NQEs induce a substantial increase in both the ionic and electronic pressures.This confirms the importance of NQEs for highly accurate equation-of-state data on highly driven hydrogen.For Te>20 kK,increasing Te in the warm dense hydrogen has slight effects on the ionic radial distribution function and equation of state in the range of densities considered.In addition,we confirm that compared with thermostatted ring-polymer molecular dynamics,the primitive PIMD algorithm overestimates electronic pressures,a consequence of the overly localized ionic description from the primitive scheme.
文摘The triple bond in N_(2)has an extremely high bond energy and is thus difficult to break.N_(2)is commonly converted into NH3 artificially via the Haber-Bosch process,and NH_(3)can be utilized to produce other nitrogen-containing chemicals.Here,we developed an electron catalyzed method to directly fix N_(2)into azos,by pushing and pulling the electron into and from the aromatic halide with the cyclic voltammetry method.The round-trip journey of electron can successfully weaken the triple bond in N_(2)through the electron pushing-induced aryl radical via a“brick trowel”transition state,and then produce the diazonium ions by pulling the electron out from the diazo radical intermediate.Different azos can be synthesized with this developed electron catalyzed approach.This approach provides a novel concept and practical route for the fixation of N_(2)at atmospheric pressure into chemical products valuable for industrial and commercial applications.
基金This work is supported by National Natural Science Foundation of China(No.42372054)。
文摘The features of optical defects in a chemical vapor deposition (CVD) synthetic type Ⅱ a diamond were characterized using photoluminescence (PL) spectroscopy, before and after electron irradiation. The sample was cut within a {100} growth layer, and irradiated with 2 MeV electrons along the <100> axis. PL spectra of sample were collected under 532 nm and 355 nm laser excitation, at room temperature and 77 K, and linear scanning analysis along incident depth was applied to determine the distribution of defects. The pre-irradiation characterization results revealed uniformly distributed PL centers at 389 nm, 469 nm, 533 nm, 575 nm (ZPL of NV 0), 637 nm (ZPL of NV -), and 736.7/737.1 nm (ZPL doublet of SiV -). After irradiation, the differential responses of these as-grown defects were observed, alongside the emergence of irradiation-induced defects, namely 489 nm center, H3 center (ZPL at 504 nm) and GR1 center (ZPL at 741 nm). The maximum penetration depth of 2 MeV electron-irradiation induced defects was determined to be 2.1 mm. This work primarily presents the depth profiles of both as-grown and irradiation-induced defects in 2 MeV electrons irradiated diamond. The result provides experimental data for better understanding of the radiation effect in diamonds. Serving as a reference for diamond enhancement by electron irradiation.
基金supported by the National Natural Science Foundation of China(No.22273006).
文摘The gold nano-plates(Au NPLs)have been extensively studied for their high quality factor as mechanical resonators.But it remains still unclear how the thickness and morphology of Au NPLs affect the hot electron diffusion.Here we have employed transient absorption microscopy to gain spatiotemporal imaging of the hot electron diffusion in Au NPLs.Au NPLs of varying thickness over 200 nm were synthesized.It was found that the hot electron diffusion of Au NPL excited at the boundary is obviously faster than that excited at the internal surface.And thinner Au NPLs exhibit a faster hot electron diffusion rate compared to thicker Au NPLs.Because the time constant of hot electron cooling(electron-phonon coupling)is independent of the excited position and thickness of Au NPLs,the effect of electron-phonon coupling on hot electron diffusion should be ruled out.So the hot electron diffusion rate is highly dimensionality-dependent.The quasi-one-dimensional diffusion along the boundary of nanoplate has the fastest rate of 50 cm^(2)/s,and the three-dimensional diffusion has the slowest rate of 22 cm^(2)/s.The fundamental investigation on the hot electrons transport property of Au NPLs offers a new insight for designing metal-based optoelectronic devices.
文摘The propagation properties of ion-acoustic solitary and shock waves in the magnetized viscous plasma with nonthermal trapped electrons are investigated.The Cairns-Gurevich distribution as the electron distribution is considered to describe the plasma nonthermality and particle trapping.By adopting the reductive perturbation technique,we derived the nonlinear Schamel-Korteweg-de Vries-Burgers(SKdVB)equation,and then obtained the ion-acoustic shock and solitary wave solutions of the SKdVB equation for different limiting cases.It is found that the impact of nonthermal parameterα,external magnetic fieldΩ,obliqueness lz,wave speed U0,and the ion kinematic viscosityη0can significantly change the characteristics of the shock and solitary waves.These results may be useful for better understanding the propagation of nonlinear structures in space(i.e.Earth's magnetosphere and ionosphere,auroral regions)and laboratory plasma with nonthermal trapped electrons.
基金supported by the National Natural Science Foundation of China(22179034,22279030)the Natural Science Foundation of Heilongjiang Province(ZD2023B002).
文摘The susceptibility of Pt catalyst surfaces to carbon monoxide(CO)poisoning in anodic hydrogen oxidation reaction(HOR)has been a critical constraint on the development of proton exchange membrane fuel cells(PEMFCs).Effectively regulating the electronic structure of Pt to enhance CO resistance is crucial for developing high-performance catalysts with robust anti-poisoning capabilities.Herein,the Pt/W@NCNF featured by Pt nanoparticles and atomical dispersed tungsten(W)sites on N-doped carbon nanofibers is developed for CO tolerance HOR catalyst.The presence of W enables the electron transfer from Pt,which promotes electron rearrangement in the Pt-5d orbitals.It not only optimizes the adsorption of H^(*) and CO^(*)on Pt,but also the OH^(*) intermediates adsorbed on the W sites oxidize the CO*adsorbed on Pt,thereby retaining more active sites for H_(2) adsorption and oxidation.The HOR exchange current density of Pt/W@NCNF reaches 1.35 times that of commercial Pt/C,and the limiting current density decreases by only 3.4%after introducing 1000 ppm CO in H_(2).Notably,the Pt/W@NCNF-based PEMFCs deliver markedly superior performance across a range of CO concentrations.The present study demonstrates that electronic modulation of Pt is an effective strategy for simultaneously achieving resistance to CO and promoted HOR activity.
基金supported by the National Natural Science Foundation of China(52172170)Guangdong Natural Science Foundation for Distinguished Young Scholars(2023B1515020114)+2 种基金Fundamental Research Funds for the Central Universities(24lgqb003)Guangdong University Innovation and Enhancement Program(2024KTSCX003)Science and Technology Projects of Guangzhou(2025A04J4230).
文摘Stretchable electronics have been recognized as intriguing next-generation electronics that possess huge market value,and stretchable electronic conductors(SECs)are essential for stretchable electronics,which not only can serve as critical functional components but also are the indispensable electronic connections bridging various electronic components within stretchable electronic systems.Herein,we offer a comprehensive review of recent progress in SECs including the material categories,structure designs,fabrication techniques,and applications.The characteristics,performance enhancement strategies,and application requirements are emphasized.Based on the recent advances,the existing challenges and future prospects are outlined and discussed.
基金supported in part by the National Key R&D Program of China under Grant 2024YFB4405300 and 2022YFA1204300the Natural Science Foundation of Hunan Province under Grant 2023JJ20016+2 种基金the National Natural Science Foundation of China under Grants of 52221001 and 62090035the Key Research and Development Plan of Hunan Province under grants of 2022GK3002 and 2023GK2012the Key Program of Science and Technology Department of Hunan Province under grant of 2020XK2001。
文摘Permeable electronics promise improved physiological comfort,but remain constrained by limited functional integration and poor mechanical robustness.Here,we report a three-dimensional(3D)permeable electronic system that overcomes these challenges by combining electrospun SEBS nanofiber mats,high-resolution liquid metal conductors patterned via thermal imprinting(50μm),and a strain isolators(SIL)that protects vertical interconnects(VIAs)from stress concentration.This architecture achieves ultrahigh air permeability(>5.09 m L cm^(-2)min^(-1)),exceptional stretchability(750%fracture strain),and reliable conductivity maintained through more than 32,500 strain cycles.Leveraging these advances,we have integrated multilayer circuits,strain sensors,and a three-axis accelerometer to achieve a fully integrated,stretchable,permeable wireless real-time gesture recognition glove.The system enables accurate sign language interpretation(98%)and seamless robotic hand control,demonstrating its potential for assistive technologies.By uniting comfort,durability,and high-density integration,this work establishes a versatile platform for nextgeneration wearable electronics and interactive human-robot interfaces.
基金supported by the National Natural Science Foundation of China(Grant Nos.11804348,11775056,11975154,12225505,and 12405281)the Science Challenge(Project No.TZ2018005)+2 种基金supported by the Shanghai Pujiang Program(Grant No.23PJ1414600)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB0890203)supported by the Accelerator Technology Helmholtz Infrastructure consortium ATHENA.
文摘The effects of initial spin orientation on the final electron beam polarization in laser wakefield acceleration in a pre-polarized plasma are investigated theoretically and numerically.From the results of variation of the initial spin direction,the spin dynamics of the electron beam are found to depend on the self-injection mechanism.The effects of wakefields and laser fields are studied using test particle dynamics and particle-in-cell simulations based on the Thomas-Bargmann-Michel-Telegdi equation.Compared with transverse injection,longitudinal injection is found to be preferable for obtaining a highly polarized electron beam.
基金supported by the National Key R&D Program of China(Grant No.2023YFA1406200)the National Natural Science Foundation of China(Grant Nos.12374004 and 12174141)the High Performance Computing Center of Jilin University,China。
文摘The discovery of pressure-induced superconducting electrides has sparked a intense wave of interest in novel superconductors.However,opinions vary regarding the relationship between non-nuclear attractors(NNAs)and superconductivity,with two opposing views currently represented by the materials Li_(6)P and Li_(6)C.Here,we choose the ternary Li–C–P as a model system and reveal the underlying mechanism by which NNAs contribute to superconductivity.The loosely bound NNAs in the superlithide Li_(14)CP covalently bond with Li and form unique satellite interstitial electrons(SIEs)around Li near the Fermi level,dominating the superconductivity.First-principles calculations show that the SIEs progressively increase in number and couple strongly with phonons at high pressure.Moreover,the Fermi surface nesting associated with SIEs induces phonon softening,further enhancing the electron–phonon coupling and giving the superlithide Li_(14)CP a T_(c)of 10.6 K at 300 GPa.The leading role of SIEs in superconductivity is a general one and is also relevant to the recently predicted Li_(6)P and Li_(6)C.Our work presented here reshapes the understanding of NNA-dominated superconductivity and holds promise for guiding future discoveries and designs of novel high-temperature superconductors.
基金supported by the Advanced Materials-National Science and Technology Major Project(Grant No.2025ZD0618401)the National Natural Science Foundation of China(Grant No.12504285)+1 种基金the Natural Science Foundation of Jiangsu Province(Grant No.BK20250472)NFSG grant from BITS-Pilani,Dubai campus。
文摘The rapid advancement of machine learning based tight-binding Hamiltonian(MLTB)methods has opened new avenues for efficient and accurate electronic structure simulations,particularly in large-scale systems and long-time scenarios.This review begins with a concise overview of traditional tight-binding(TB)models,including both(semi-)empirical and first-principles approaches,establishing the foundation for understanding MLTB developments.We then present a systematic classification of existing MLTB methodologies,grouped into two major categories:direct prediction of TB Hamiltonian elements and inference of empirical parameters.A comparative analysis with other ML-based electronic structure models is also provided,highlighting the advancement of MLTB approaches.Finally,we explore the emerging MLTB application ecosystem,highlighting how the integration of MLTB models with a diverse suite of post-processing tools from linear-scaling solvers to quantum transport frameworks and molecular dynamics interfaces is essential for tackling complex scientific problems across different domains.The continued advancement of this integrated paradigm promises to accelerate materials discovery and open new frontiers in the predictive simulation of complex quantum phenomena.
基金supported by the Key R&D Program of Shandong Province(No.2023SFGC0101)Shandong Excellent Young Scientists Fund Program(Overseas)(No.2023HWYQ-047)+1 种基金the Natural Science Foundation of Shandong Province(No.ZR2022QA039)the National Natural Science Foundation of China(NSFC)(No.U2106202).
文摘Traditional digitizers for signal readout of PET detectors are based on commercial analog-to-digital converters(ADC).However,the cost and power consumption of an entire electronic readout system based on digitizers for a PET scanner are high.To address this problem,a soft-core ADC based on a field-programmable gate array(FPGA)was proposed.An FPGA-based ADC(FPGA-ADC)combines low loss and high performance.To achieve good performance,the FPGA-ADC requires three calibrations:time-to-digital converter(TDC)length calibration,TDC alignment calibration,and TDC-to-ADC calibration.A prototype front-end electronics based on FPGA-ADC was built to evaluate the performance of time-of-flight positron emission tomography(TOF PET)detectors.Each PET detector consists of a LYSO crystal single-ended coupled to a silicon photomultiplier(SiPM).The experimental results show that the full-width at half-maximum(FWHM)energy resolution for 511 keV gamma photons after saturation correction of the SiPM was 12.3%.The FWHM coincidence timing resolution(CTR)of the TOF PET detector with the readout of the front-end electronic prototype is 385.2 ps.FPGA-ADCbased front-end electronics are very promising for multichannel,low-cost,highly integrated,and power-efficient readout electronic systems for radiation detector applications.
基金supported by the National Natural Science Foundation of China(22074072,22274083,52376199)the Shandong Provincial Natural Science Foundation(ZR2023LZY005)+1 种基金the Exploration Project of the State Key Laboratory of BioFibers and EcoTextiles of Qingdao University(TSKT202101)the Fundamental Research Funds for the Central Universities(2022BLRD13,2023BLRD01).
文摘A rapidly growing field is piezoresistive sensor for accurate respiration rate monitoring to suppress the worldwide respiratory illness.However,a large neglected issue is the sensing durability and accuracy without interference since the expiratory pressure always coupled with external humidity and temperature variations,as well as mechanical motion artifacts.Herein,a robust and biodegradable piezoresistive sensor is reported that consists of heterogeneous MXene/cellulose-gelation sensing layer and Ag-based interdigital electrode,featuring customizable cylindrical interface arrangement and compact hierarchical laminated architecture for collectively regulating the piezoresistive response and mechanical robustness,thereby realizing the long-term breath-induced pressure detection.Notably,molecular dynamics simulations reveal the frequent angle inversion and reorientation of MXene/cellulose in vacuum filtration,driven by shear forces and interfacial interactions,which facilitate the establishment of hydrogen bonds and optimize the architecture design in sensing layer.The resultant sensor delivers unprecedented collection features of superior stability for off-axis deformation(0-120°,~2.8×10^(-3) A)and sensing accuracy without crosstalk(humidity 50%-100%and temperature 30-80).Besides,the sensor-embedded mask together with machine learning models is achieved to train and classify the respiration status for volunteers with different ages(average prediction accuracy~90%).It is envisioned that the customizable architecture design and sensor paradigm will shed light on the advanced stability of sustainable electronics and pave the way for the commercial application in respiratory monitory.
基金supported by the Hundred-person Program of Chinese Academy of Sciences and the National Natural Science Foundation of China(No.11905074).
文摘Electron beam injectors are pivotal components of large-scale scientific instruments,such as synchrotron radiation sources,free-electron lasers,and electron-positron colliders.The quality of the electron beam produced by the injector critically influences the performance of the entire accelerator-based scientific research apparatus.The injectors of such facilities usually use photocathode and thermionic-cathode electron guns.Although the photocathode injector can produce electron beams of excellent quality,its associated laser system is massive and intricate.The thermionic-cathode electron gun,especially the gridded electron gun injector,has a simple structure capable of generating numerous electron beams.However,its emittance is typically high.In this study,methods to reduce beam emittance are explored through a comprehensive analysis of various grid structures and preliminary design results,examining the evolution of beam phase space at different grid positions.An optimization method for reducing the emittance of a gridded thermionic-cathode electron gun is proposed through theoretical derivation,electromagnetic-field simulation,and beam-dynamics simulation.A 50%reduction in emittance was achieved for a 50 keV,1.7 A electron gun,laying the foundation for the subsequent design of a high-current,low-emittance injector.
基金supported by the introduction of Talent Research Fund in Nanjing Institute of Technology(YKJ202204)the National Natural Science Foundation of China(52401282 and 52300206)the Natural Science Foundation of Jiangsu Province(BK20230701 and BK20230705).
文摘Achieving high-energy density remains a key objective for advanced energy storage systems.However,challenges,such as poor cathode conductivity,anode dendrite formation,polysulfide shuttling,and electrolyte degradation,continue to limit performance and stability.Molecular and ionic dipole interactions have emerged as an effective strategy to address these issues by regulating ionic transport,modulating solvation structures,optimizing interfacial chemistry,and enhancing charge transfer kinetics.These interactions also stabilize electrode interfaces,suppress side reactions,and mitigate anode corrosion,collectively improving the durability of high-energy batteries.A deeper understanding of these mechanisms is essential to guide the design of next-generation battery materials.Herein,this review summarizes the development,classification,and advantages of dipole interactions in high-energy batteries.The roles of dipoles,including facilitating ion transport,controlling solvation dynamics,stabilizing the electric double layer,optimizing solid electrolyte interphase and cathode–electrolyte interface layers,and inhibiting parasitic reactions—are comprehensively discussed.Finally,perspectives on future research directions are proposed to advance dipole-enabled strategies for high-performance energy storage.This review aims to provide insights into the rational design of dipole-interactive systems and promote the progress of electrochemical energy storage technologies.
基金supported by the National Natural Science Foundation of China(No.12305385)Key Projects of Scientific Research of the Hunan Provincial Department of Education(22A0310)the Research Startup Project of University of South China(220XQD025).
文摘In this study,the dosimetric characteristics(thickness applicability,preheating time,temperature and humidity dependence,in-batch uniformity,readout reproducibility,dose linearity,self-decay,and electron energy response)of engineered polycarbonate films irradiated with an electron beam(0–600 kGy)were investigated using photoluminescence spectroscopy.The results show a linear relationship between photoluminescence intensity and radiation dose when the thickness of the polycarbonate film is 0.3 mm.A higher fluorescence intensity can be obtained by preheating at 60℃ for 180 min before photoluminescence spectrum analysis.As the temperature during spectral testing and the ambient humidity(during and after irradiation)increased,the photoluminescence intensity of the polycarbonate films decreased.The photoluminescence intensity deviation of the polycarbonate films produced within the same batch at 100 kGy is 2.73%.After ten times of repeated excitations and readouts,the coefficients of variation in photoluminescence intensity are less than 8.6%,and the linear correlation coefficient between photoluminescence intensity and irradiation dose is 0.965 in the dose capture range of 20–600 kGy.Within 60 days of irradiation,the photoluminescence intensity of the polycarbonate film decreased to 60%of the initial value.The response of the 0.3 mm polycarbonate films to electron beams with energies exceeding 3.5 MeV does not differ significantly.This comprehensive analysis indicates the potential of polycarbonate films as a high-radiation dose detection material.
基金supported by the National Key R&D Program of China (Grant No.2022YFA1403201)the National Natural Science Foundation of China (Grant Nos.12125404,T2495231,123B2049,and 12204138)+9 种基金the Advanced MaterialsNational Science and Technology Major Project (Grant No.2024ZD0607000)the Natural Science Foundation of Jiangsu Province (Grant Nos.BK20233001 and BK20253009)the Jiangsu Funding Program for Excellent Postdoctoral Talent (Grant No.2024ZB002)the China Postdoctoral Science Foundation (Grant No.2025M773331)the Fundamental and Interdisciplinary Disciplines Breakthrough Plan of the Ministry of Education of Chinathe AI&AI for Science program of Nanjing UniversityArtificial Intelligence and Quantum physics (AIQ) program of Nanjing Universitythe Fundamental Research Funds for the Central Universitiesthe Natural Science Foundation of Nanjing University of Posts and Telecommunications(Grant Nos.NY224165,NY220038,and NY219087)the Hua Li Talents Program of Nanjing University of Posts and Telecommunications。
文摘We report a theoretical investigation into superconductivity within the MAXH_(6) quaternary hydride system using first-principles calculations,where M and A denote alkali and alkaline earth elements,respectively,and X represents transition metal elements.Systematic analysis of electronic band structures,phonon dispersions,and electron-phonon coupling reveals that substitution of MA binary metal combinations and X metal atoms can create favorable conditions for superconductivity.Mapping of superconducting critical temperatures,combined with dynamical stability analysis through phonon calculations,identifies ten superconducting candidates at ambient pressure.Among these,LiNaAgH_(6) exhibits nearly-free-electron behavior reminiscent of monovalent electron superconductors.It demonstrates exceptional superconducting properties with electron–phonon coupling λ=2.707,which yields a superconducting transition temperature T_(c) of 206.4 K using the Allen–Dynes formula.Its structural analogs MgNaPdH_(6),LiMgPdH_(6),LiMgAgH_(6),LiMgAuH_(6) all exhibit superconducting transition temperatures above 110 K.These findings advance our fundamental understanding of superconductivity in quaternary hydrides and provide guidance for rational design of new high-temperature superconducting materials.