Hafnia-based ferroelectrics have emerged as promising materials for next-generation nanoelectronics owing to their robust nanoscale properties and compatibility with metal-oxide-semiconductor technology.However,their ...Hafnia-based ferroelectrics have emerged as promising materials for next-generation nanoelectronics owing to their robust nanoscale properties and compatibility with metal-oxide-semiconductor technology.However,their metastable nature remains a key challenge for practical implementation.Utilizing scanning transmission electron microscopy,we investigated the atomic-scale mechanisms governing ferroelectric transitions and the metastability of polar phases in 10-nm-thick Hf_(0.5)Zr_(0.5)O_(2)thin films.Our results demonstrate that oxygen vacancies,coupled with rhombohedral distortions of the cation lattice,facilitate ferroelectric phase transitions and enable robust polar switching through adaptive processes,including cell-by-cell oxygen displacement and domain-wall-mediated nucleation and growth.These findings underscore the pivotal role of oxygen vacancies and lattice distortions in stabilizing polar phases and provide detailed insights into the atomic structures and transition dynamics of polymorphic Hf_(0.5)Zr_(0.5)O_(2-x),thereby advancing its potential for practical device applications.展开更多
As an advanced device for observing atmospheric winds,the spaceborne Doppler Asymmetric Spatial Heterodyne(DASH)interferometer also encounters challenges associated with phase distortion,par-ticularly in limb sounding...As an advanced device for observing atmospheric winds,the spaceborne Doppler Asymmetric Spatial Heterodyne(DASH)interferometer also encounters challenges associated with phase distortion,par-ticularly in limb sounding scenarios.This paper discusses interferogram modeling and phase distortion cor-rection techniques for spaceborne DASH interferometers.The modeling of phase distortion interferograms with and without Doppler shift for limb observation was conducted,and the effectiveness of the analytical expression was verified through numerical simulation.The simulation results indicate that errors propagate layer by layer while using the onion-peeling inversion algorithm to handle phase-distorted interferograms.In contrast,the phase distortion correction algorithm can achieve effective correction.This phase correction method can be successfully applied to correct phase distortions in the interferograms of the spaceborne DASH interferometer,providing a feasible solution to enhance its measurement accuracy.展开更多
The conversion of CO_(2)to dimethyl carbonate(DMC)offers a promising route for CO_(2)utilization.In this study,four CeO2 catalysts with distinct nanostructures were synthesized via a template-free hydrothermal method ...The conversion of CO_(2)to dimethyl carbonate(DMC)offers a promising route for CO_(2)utilization.In this study,four CeO2 catalysts with distinct nanostructures were synthesized via a template-free hydrothermal method by systematically varying the types and concentrations of precipitants as well as the hydrothermal reaction conditions,and they were employed for DMC synthesis from CO_(2)and methanol.The atomic arrangements of CeO_(2)varied significantly with its morphology,leading to differences in lattice distortion,which directly influenced the concentration of oxygen vacancies.Notably,the CeO_(2)nanospheres,which exhibited the highest lattice distortion and oxygen vacancy concentration,achieved a DMC yield(11.12 mmol/g)48 times greater than that of the nanocubes(0.23 mmol/g).The results indicated that oxygen vacancies played a pivotal role in the catalytic process by facilitating the adsorption and activation of CO_(2)to form bidentate carbonates,as well as activating methanol to generate methoxy species.These processes collectively promoted the formation of the key intermediate(*CH3OCOO).This study proposes a strategy to enhance the oxygen vacancy concentration by increasing lattice distortion,providing valuable insights for designing high-performance CeO_(2)catalysts for DMC synthesis.展开更多
Collecting amounts of distorted/clean image pairs in the real world is non-trivial,which severely limits the practical application of these supervised learning-based methods to real-world image super-resolution(RealSR...Collecting amounts of distorted/clean image pairs in the real world is non-trivial,which severely limits the practical application of these supervised learning-based methods to real-world image super-resolution(RealSR).Previous works usually address this problem by leveraging unsupervised learning-based technologies to alleviate the dependency on paired training samples.However,these methods typically suffer from unsatisfactory texture synthesis due to the lack of supervision of clean images.To overcome this problem,we are the first to take a close look at the under-explored direction for RealSR,i.e.,few-shot real-world image super-resolution,which aims to tackle the challenging RealSR problem with few-shot distorted/clean image pairs.Under this brand-new scenario,we propose distortion relation guided transfer learning(DRTL)for the few-shot RealSR by transferring the rich restoration knowledge from auxiliary distortions(i.e.,synthetic distortions)to the target RealSR under the guidance of the distortion relation.Concretely,DRTL builds a knowledge graph to capture the distortion relation between auxiliary distortions and target distortion(i.e.,real distortions in RealSR).Based on the distortion relation,DRTL adopts a gradient reweighting strategy to guide the knowledge transfer process between auxiliary distortions and target distortions.In this way,DRTL is able to quickly learn the most relevant knowledge from the synthetic distortions for the target distortion.We instantiate DRTL with two commonly-used transfer learning paradigms,including pretraining and meta-learning pipelines,to realize a distortion relation-aware few-shot RealSR.Extensive experiments on multiple benchmarks and thorough ablation studies demonstrate the effectiveness of our DRTL.展开更多
The traditional orbit determination method based on pulsar profile distortion can determine the six elements of the orbit.However,the estimation accuracies of these methods are limited and the computational load of a ...The traditional orbit determination method based on pulsar profile distortion can determine the six elements of the orbit.However,the estimation accuracies of these methods are limited and the computational load of a six-dimensional search is huge.To solve this problem,the differential-geometry-based Multi-dimensional Joint Position-Velocity Estimation(MJPVE)using Crab pulsar profile distortion is proposed in this paper.Firstly,through theoretical analysis,it is found that the pulsar profile distortion caused by the initial state error in some joint positionvelocity directions is very small.In other words,the accuracies of estimation in these directions are very low.Namely,the search dimension can be reduced,which in turn greatly reduces the computational load.Then,we construct the chi-squared function of the pulsar profile with respect to the estimation error in joint position-velocity direction and use differential geometry to find the joint position-velocity directions corresponding to different degrees of distortion.Finally,we utilize the grid search based on directory folding in these joint position-velocity directions corresponding to large degrees of distortion to obtain the joint position-velocity estimation.The experimental results show that compared with the grouping bi-chi-squared inversion method,MJPVE has high precision and extensive navigation information.展开更多
Strong-field terahertz(THz) radiation holds significant potential in non-equilibrium state manipulation, electron acceleration, and biomedical effects. However, distortion-free detection of strong-field THz waveforms ...Strong-field terahertz(THz) radiation holds significant potential in non-equilibrium state manipulation, electron acceleration, and biomedical effects. However, distortion-free detection of strong-field THz waveforms remains an essential challenge in THz science and technology. To address this issue, we propose a ferromagnetic detection scheme based on Zeeman torque sampling, achieving distortion-free strong-field THz waveform detection in Py films. Thickness-dependent characterization(3–21 nm) identifies peak detection performance at 21 nm within the investigated range. Furthermore, by structurally engineering the Py ferromagnetic layer, we demonstrate strong-field THz detection in symmetric Ta(3 nm)/Py(9 nm)/Ta(3 nm) heterostructure while simultaneously resolving Zeeman torque responses and collective spin-wave dynamics in asymmetric W(4 nm)/Py(9 nm)/Pt(2 nm)heterostructure. We calculated spin wave excitations and spin orbit torque distributions in asymmetric heterostructures, along with spin wave excitations in symmetric modes. This approach overcomes the sensitivity limitations of conventional techniques in strong-field conditions.展开更多
Fe-N-C catalysts are promising substitutes for precious-metal platinum in acidic oxygen reduction reactions(ORR),yet their moderate intrinsic activity and susceptibility to reactive oxygen species(ROS)-induced degrada...Fe-N-C catalysts are promising substitutes for precious-metal platinum in acidic oxygen reduction reactions(ORR),yet their moderate intrinsic activity and susceptibility to reactive oxygen species(ROS)-induced degradation hinder practical implementation.Herein,we fabricate a Ru-Fe dual-site catalyst(RuFe-N-C)through a two-step pyrolysis strategy.Structural characterization reveals atomic-scale proximity between Ru single atoms and Fe-N_(4) moieties,exhibiting a projected distance of~1.7Å.This configuration induces Fe–N bond elongation accompanied by 2.5%lattice distortion.The optimized RuFe-N-C catalyst exhibits high ORR performance,with a half-wave potential(E_(1/2))of 0.840 V and peak power density(P_(max))of 938 mW cm^(-2) under 150 kPa absolute H_(2)-O_(2).These metrics signify substantial enhancements relative to conventional Fe-N-C benchmarks(+21 mV in E_(1/2) and+42%in P_(max)).Moreover,the catalyst maintains outstanding stability,showing merely 17 mV E_(1/2) decay after 10000 accelerated durability test(ADT)cycles.Experimental analyses reveal a bifunctional mechanism:(1)Adjacent Ru sites substantially enhance the intrinsic ORR activity of Fe-N_(4) moieties,delivering a notable turnover frequency(TOF=17.86 e site^(-1) s^(-1) at 0.85 V vs.RHE)that exceeds state-of-the-art Fe-N-C benchmarks by 1-2 orders of magnitude(<1 e site^(-1) s^(-1));(2)Ru centers function as electron relays that facilitate ROS scavenging,thus suppressing degradation.This work establishes a paradigm for engineering bimetallic single-atom catalysts through synergistic electronic modulation to concurrently enhance activity and stability.展开更多
Efficient and stable electrocatalysts are essential for seawater splitting to sustain electrolysis without chloride corrosion,particularly at the anode.Furthermore,the oxygen evolution reaction(OER)requires high overp...Efficient and stable electrocatalysts are essential for seawater splitting to sustain electrolysis without chloride corrosion,particularly at the anode.Furthermore,the oxygen evolution reaction(OER)requires high overpotential due to the universal scaling relationship.Herein,molybdenum doping FeNi_(2)Se_(4)with lattice distortion is proposed to break the scaling relationship.Mo-FeNi_(2)Se_(4)shows high performance in direct seawater electrolysis and achieves current densities of 10 and 100 mA cm^(−2) at overpotentials of 190 and 250 mV,respectively,together with high OER selectivity and long-term stability.It is found that the lattice distortion induced by Mo doping in(3 1 0)plane of FeNi_(2)Se_(4),leads to a decrease in the d-band center and the adsorption energy of ^(*)O,which not only breaks the scaling relationship of OER but also lowers the energy barriers of rate-determining step.Moreover,it enhances the corrosion resistance to Cl^(−),and realizes the high-efficiency seawater electrolysis driven by photovoltaic.展开更多
The estimation of orientation parameters and correction of lens distortion are crucial problems in the field of Unmanned Aerial Vehicles(UAVs)photogrammetry.In recent years,the utilization of UAVs for aerial photogram...The estimation of orientation parameters and correction of lens distortion are crucial problems in the field of Unmanned Aerial Vehicles(UAVs)photogrammetry.In recent years,the utilization of UAVs for aerial photogrammetry has witnessed a surge in popularity.Typically,UAVs are equipped with low-cost non-metric cameras and a Position and Orientation System(POS).Unfortunately,the Interior Orientation Parameters(IOPs)of the non-metric cameras are not fixed.Whether the lens distortions are large or small,they effect the image coordinates accordingly.Additionally,Inertial Measurement Units(IMUs)often have observation errors.To address these challenges and improve parameter estimation for UAVs Light Detection and Ranging(LiDAR)and photogrammetry,this paper analyzes the accuracy of POS observations obtained from Global Navigation Satellite System Real Time Kinematic(GNSS-RTK)and IMU data.A method that incorporates additional known conditions for parameter estimation,a series of algorithms to simultaneously solve for IOPs,Exterior Orientation Parameters(EOPs),and camera lens distortion correction parameters are proposed.Extensive experiments demonstrate that the coordinates measured by GNSS-RTK can be directly used as linear EOPs;however,angular EOP measurements from IMUs exhibit relatively large errors compared to adjustment results and require correction during the adjustment process.The IOPs of non-metric cameras vary slightly between images but need to be treated as unknown parameters in high precision applications.Furthermore,it is found that the Ebner systematic error model is sensitive to the choice of the magnification parameter of the photographic baseline length in images,it should be set as less than or equal to one third of the photographic baseline to ensure stable solutions.展开更多
To eliminate distortion caused by vertical drift and illusory slopes in atomic force microscopy(AFM)imaging,a lifting-wavelet-based iterative thresholding correction method is proposed in this paper.This method achiev...To eliminate distortion caused by vertical drift and illusory slopes in atomic force microscopy(AFM)imaging,a lifting-wavelet-based iterative thresholding correction method is proposed in this paper.This method achieves high-quality AFM imaging via line-by-line corrections for each distorted profile along the fast axis.The key to this line-by-line correction is to accurately simulate the profile distortion of each scanning row.Therefore,a data preprocessing approach is first developed to roughly filter out most of the height data that impairs the accuracy of distortion modeling.This process is implemented through an internal double-screening mechanism.A line-fitting method is adopted to preliminarily screen out the obvious specimens.Lifting wavelet analysis is then carried out to identify the base parts that are mistakenly filtered out as specimens so as to preserve most of the base profiles and provide a good basis for further distortion modeling.Next,an iterative thresholding algorithm is developed to precisely simulate the profile distortion.By utilizing the roughly screened base profile,the optimal threshold,which is used to screen out the pure bases suitable for distortion modeling,is determined through iteration with a specified error rule.On this basis,the profile distortion is accurately modeled through line fitting on the finely screened base data,and the correction is implemented by subtracting the modeling result from the distorted profile.Finally,the effectiveness of the proposed method is verified through experiments and applications.展开更多
Jahn-Teller distortion(JTD)remains a fundamental bottleneck for transition metal oxides(TMOs)in electrochemical energy storage,where the e_(g)-orbital single-electron occupancy induces irreversible octahedral collapse...Jahn-Teller distortion(JTD)remains a fundamental bottleneck for transition metal oxides(TMOs)in electrochemical energy storage,where the e_(g)-orbital single-electron occupancy induces irreversible octahedral collapse and rapid capacity fading.Here,we pioneer an itinerant-electron-mediated dynamic suppression strategy that fundamentally reshapes the JTD evolution pathway throughπ-d orbital hybridization engineering.By constructing reduced graphene oxide/TMO heterointerfaces(rGO/MO_(x),M=Fe/Ni/Mn),localized 3d electrons are transformed into delocalized itinerant states,which(1)eliminate e_(g)-band degeneracy via orbital repopulation and(2)establish an electron density buffer layer to neutralize lattice strain.This electronic regulation enables ultrafast Na^(+)diffusion kinetics(508.3 F g^(−1)at 1 A g^(−1)→304.6 F g^(−1)at 20 A g^(−1))and near-zero lattice deformation(91.07%capacitance retention after 20,000 cycles).Synchrotron-based X-ray absorption spectroscopy and density functional theory calculations reveal that itinerant electron dynamics actively decouple the Mn^(3+)d^(4)electronic configuration from JTD triggering,leading to a dramatic suppression of octahedral distortion compared to the conventional MnO_(2).The proposed electron delocalization-to-lattice stabilization paradigm opens a universal route to design distortion-resistant electrodes for high-power energy storage systems.展开更多
In semiconductor quantum dot systems,pulse distortion is a significant source of coherent errors,which impedes qubit characterization and control.Here,we demonstrate two calibration methods using a two-qubit system as...In semiconductor quantum dot systems,pulse distortion is a significant source of coherent errors,which impedes qubit characterization and control.Here,we demonstrate two calibration methods using a two-qubit system as the detector to correct distortion and calibrate the transfer function of the control line.Both methods are straightforward to implement,robust against noise,and applicable to a wide range of qubit types.The two methods differ in correction accuracy and complexity.The first,coarse predistortion(CPD)method,partially mitigates distortion.The second,all predistortion(APD)method,measures the transfer function and significantly enhances exchange oscillation uniformity.Both methods use exchange oscillation homogeneity as the metric and are suitable for any qubit driven by a diabatic pulse.We believe these methods will enhance qubit characterization accuracy and operation quality in future applications.展开更多
基金supported by the National Natural Science Foundation of China (Grant Nos.12334001,52461160301,52322311,52427802,12222414)the National Key R&D Program of China (Grant Nos.2024YFA1208201,2021YFA1400500,2021YFA1400204)the Youth Innovation Promotion Association of the CAS (Grant Nos.Y2022003 and 2020009)。
文摘Hafnia-based ferroelectrics have emerged as promising materials for next-generation nanoelectronics owing to their robust nanoscale properties and compatibility with metal-oxide-semiconductor technology.However,their metastable nature remains a key challenge for practical implementation.Utilizing scanning transmission electron microscopy,we investigated the atomic-scale mechanisms governing ferroelectric transitions and the metastability of polar phases in 10-nm-thick Hf_(0.5)Zr_(0.5)O_(2)thin films.Our results demonstrate that oxygen vacancies,coupled with rhombohedral distortions of the cation lattice,facilitate ferroelectric phase transitions and enable robust polar switching through adaptive processes,including cell-by-cell oxygen displacement and domain-wall-mediated nucleation and growth.These findings underscore the pivotal role of oxygen vacancies and lattice distortions in stabilizing polar phases and provide detailed insights into the atomic structures and transition dynamics of polymorphic Hf_(0.5)Zr_(0.5)O_(2-x),thereby advancing its potential for practical device applications.
文摘As an advanced device for observing atmospheric winds,the spaceborne Doppler Asymmetric Spatial Heterodyne(DASH)interferometer also encounters challenges associated with phase distortion,par-ticularly in limb sounding scenarios.This paper discusses interferogram modeling and phase distortion cor-rection techniques for spaceborne DASH interferometers.The modeling of phase distortion interferograms with and without Doppler shift for limb observation was conducted,and the effectiveness of the analytical expression was verified through numerical simulation.The simulation results indicate that errors propagate layer by layer while using the onion-peeling inversion algorithm to handle phase-distorted interferograms.In contrast,the phase distortion correction algorithm can achieve effective correction.This phase correction method can be successfully applied to correct phase distortions in the interferograms of the spaceborne DASH interferometer,providing a feasible solution to enhance its measurement accuracy.
基金National Natural Science Foundation of China(22008166)Fundamental Research Program of Shanxi Province(202403021211029,201901D211047).
文摘The conversion of CO_(2)to dimethyl carbonate(DMC)offers a promising route for CO_(2)utilization.In this study,four CeO2 catalysts with distinct nanostructures were synthesized via a template-free hydrothermal method by systematically varying the types and concentrations of precipitants as well as the hydrothermal reaction conditions,and they were employed for DMC synthesis from CO_(2)and methanol.The atomic arrangements of CeO_(2)varied significantly with its morphology,leading to differences in lattice distortion,which directly influenced the concentration of oxygen vacancies.Notably,the CeO_(2)nanospheres,which exhibited the highest lattice distortion and oxygen vacancy concentration,achieved a DMC yield(11.12 mmol/g)48 times greater than that of the nanocubes(0.23 mmol/g).The results indicated that oxygen vacancies played a pivotal role in the catalytic process by facilitating the adsorption and activation of CO_(2)to form bidentate carbonates,as well as activating methanol to generate methoxy species.These processes collectively promoted the formation of the key intermediate(*CH3OCOO).This study proposes a strategy to enhance the oxygen vacancy concentration by increasing lattice distortion,providing valuable insights for designing high-performance CeO_(2)catalysts for DMC synthesis.
基金supported by the National Natural Science Foundation of China(623B2098,62021001,62371434)the Postdoctoral Fellowship Program of CPSF(GZC20252293)+1 种基金the China Postdoctoral Science Foundation–Anhui Joint Support Program(2024T017AH)Anhui Postdoctoral Scientific Research Program Foundation(2025A1015).
文摘Collecting amounts of distorted/clean image pairs in the real world is non-trivial,which severely limits the practical application of these supervised learning-based methods to real-world image super-resolution(RealSR).Previous works usually address this problem by leveraging unsupervised learning-based technologies to alleviate the dependency on paired training samples.However,these methods typically suffer from unsatisfactory texture synthesis due to the lack of supervision of clean images.To overcome this problem,we are the first to take a close look at the under-explored direction for RealSR,i.e.,few-shot real-world image super-resolution,which aims to tackle the challenging RealSR problem with few-shot distorted/clean image pairs.Under this brand-new scenario,we propose distortion relation guided transfer learning(DRTL)for the few-shot RealSR by transferring the rich restoration knowledge from auxiliary distortions(i.e.,synthetic distortions)to the target RealSR under the guidance of the distortion relation.Concretely,DRTL builds a knowledge graph to capture the distortion relation between auxiliary distortions and target distortion(i.e.,real distortions in RealSR).Based on the distortion relation,DRTL adopts a gradient reweighting strategy to guide the knowledge transfer process between auxiliary distortions and target distortions.In this way,DRTL is able to quickly learn the most relevant knowledge from the synthetic distortions for the target distortion.We instantiate DRTL with two commonly-used transfer learning paradigms,including pretraining and meta-learning pipelines,to realize a distortion relation-aware few-shot RealSR.Extensive experiments on multiple benchmarks and thorough ablation studies demonstrate the effectiveness of our DRTL.
基金supported in part by the National Natural Science Foundation of China(Nos.61873196,62373030,61772187)the Innovation Program for Quantum Science and Technology(No.2021ZD0303400)。
文摘The traditional orbit determination method based on pulsar profile distortion can determine the six elements of the orbit.However,the estimation accuracies of these methods are limited and the computational load of a six-dimensional search is huge.To solve this problem,the differential-geometry-based Multi-dimensional Joint Position-Velocity Estimation(MJPVE)using Crab pulsar profile distortion is proposed in this paper.Firstly,through theoretical analysis,it is found that the pulsar profile distortion caused by the initial state error in some joint positionvelocity directions is very small.In other words,the accuracies of estimation in these directions are very low.Namely,the search dimension can be reduced,which in turn greatly reduces the computational load.Then,we construct the chi-squared function of the pulsar profile with respect to the estimation error in joint position-velocity direction and use differential geometry to find the joint position-velocity directions corresponding to different degrees of distortion.Finally,we utilize the grid search based on directory folding in these joint position-velocity directions corresponding to large degrees of distortion to obtain the joint position-velocity estimation.The experimental results show that compared with the grouping bi-chi-squared inversion method,MJPVE has high precision and extensive navigation information.
基金supported by the Scientific Research Innovation Capability Support Project for Young Faculty (Grant No.ZYGXQNJSKYCXNLZCXMI3)the National Key Research and Development Program of China (Grant No.2022YFA1604402)+1 种基金the National Natural Science Foundation of China (Grant Nos.U23A6002,92250307,and 52225106)the Beijing Municipal Science and Technology Commission,Administrative Commission of Zhongguancun Science Park (Grant No.Z25110000692500)。
文摘Strong-field terahertz(THz) radiation holds significant potential in non-equilibrium state manipulation, electron acceleration, and biomedical effects. However, distortion-free detection of strong-field THz waveforms remains an essential challenge in THz science and technology. To address this issue, we propose a ferromagnetic detection scheme based on Zeeman torque sampling, achieving distortion-free strong-field THz waveform detection in Py films. Thickness-dependent characterization(3–21 nm) identifies peak detection performance at 21 nm within the investigated range. Furthermore, by structurally engineering the Py ferromagnetic layer, we demonstrate strong-field THz detection in symmetric Ta(3 nm)/Py(9 nm)/Ta(3 nm) heterostructure while simultaneously resolving Zeeman torque responses and collective spin-wave dynamics in asymmetric W(4 nm)/Py(9 nm)/Pt(2 nm)heterostructure. We calculated spin wave excitations and spin orbit torque distributions in asymmetric heterostructures, along with spin wave excitations in symmetric modes. This approach overcomes the sensitivity limitations of conventional techniques in strong-field conditions.
文摘Fe-N-C catalysts are promising substitutes for precious-metal platinum in acidic oxygen reduction reactions(ORR),yet their moderate intrinsic activity and susceptibility to reactive oxygen species(ROS)-induced degradation hinder practical implementation.Herein,we fabricate a Ru-Fe dual-site catalyst(RuFe-N-C)through a two-step pyrolysis strategy.Structural characterization reveals atomic-scale proximity between Ru single atoms and Fe-N_(4) moieties,exhibiting a projected distance of~1.7Å.This configuration induces Fe–N bond elongation accompanied by 2.5%lattice distortion.The optimized RuFe-N-C catalyst exhibits high ORR performance,with a half-wave potential(E_(1/2))of 0.840 V and peak power density(P_(max))of 938 mW cm^(-2) under 150 kPa absolute H_(2)-O_(2).These metrics signify substantial enhancements relative to conventional Fe-N-C benchmarks(+21 mV in E_(1/2) and+42%in P_(max)).Moreover,the catalyst maintains outstanding stability,showing merely 17 mV E_(1/2) decay after 10000 accelerated durability test(ADT)cycles.Experimental analyses reveal a bifunctional mechanism:(1)Adjacent Ru sites substantially enhance the intrinsic ORR activity of Fe-N_(4) moieties,delivering a notable turnover frequency(TOF=17.86 e site^(-1) s^(-1) at 0.85 V vs.RHE)that exceeds state-of-the-art Fe-N-C benchmarks by 1-2 orders of magnitude(<1 e site^(-1) s^(-1));(2)Ru centers function as electron relays that facilitate ROS scavenging,thus suppressing degradation.This work establishes a paradigm for engineering bimetallic single-atom catalysts through synergistic electronic modulation to concurrently enhance activity and stability.
基金financially supported by the National Natural Science Foundation of China(Nos.22471289,22478430,22101300,and 22275210)Shandong Natural Science Foundation(Nos.ZR2022ME105 and ZR2023ME004)+1 种基金Qingdao Natural Science Foundation(No.23-2-1-232-zyyd-jch)the Fundamental Research Funds for the Central Universities(Nos.22CX03010A,and 22CX01002A-1).
文摘Efficient and stable electrocatalysts are essential for seawater splitting to sustain electrolysis without chloride corrosion,particularly at the anode.Furthermore,the oxygen evolution reaction(OER)requires high overpotential due to the universal scaling relationship.Herein,molybdenum doping FeNi_(2)Se_(4)with lattice distortion is proposed to break the scaling relationship.Mo-FeNi_(2)Se_(4)shows high performance in direct seawater electrolysis and achieves current densities of 10 and 100 mA cm^(−2) at overpotentials of 190 and 250 mV,respectively,together with high OER selectivity and long-term stability.It is found that the lattice distortion induced by Mo doping in(3 1 0)plane of FeNi_(2)Se_(4),leads to a decrease in the d-band center and the adsorption energy of ^(*)O,which not only breaks the scaling relationship of OER but also lowers the energy barriers of rate-determining step.Moreover,it enhances the corrosion resistance to Cl^(−),and realizes the high-efficiency seawater electrolysis driven by photovoltaic.
基金Natural Science Foundation of Hunan Province,China(No.2024JJ8335)Open Topic of Hunan Geospatial Information Engineering and Technology Research Center,China(No.HNGIET2023004).
文摘The estimation of orientation parameters and correction of lens distortion are crucial problems in the field of Unmanned Aerial Vehicles(UAVs)photogrammetry.In recent years,the utilization of UAVs for aerial photogrammetry has witnessed a surge in popularity.Typically,UAVs are equipped with low-cost non-metric cameras and a Position and Orientation System(POS).Unfortunately,the Interior Orientation Parameters(IOPs)of the non-metric cameras are not fixed.Whether the lens distortions are large or small,they effect the image coordinates accordingly.Additionally,Inertial Measurement Units(IMUs)often have observation errors.To address these challenges and improve parameter estimation for UAVs Light Detection and Ranging(LiDAR)and photogrammetry,this paper analyzes the accuracy of POS observations obtained from Global Navigation Satellite System Real Time Kinematic(GNSS-RTK)and IMU data.A method that incorporates additional known conditions for parameter estimation,a series of algorithms to simultaneously solve for IOPs,Exterior Orientation Parameters(EOPs),and camera lens distortion correction parameters are proposed.Extensive experiments demonstrate that the coordinates measured by GNSS-RTK can be directly used as linear EOPs;however,angular EOP measurements from IMUs exhibit relatively large errors compared to adjustment results and require correction during the adjustment process.The IOPs of non-metric cameras vary slightly between images but need to be treated as unknown parameters in high precision applications.Furthermore,it is found that the Ebner systematic error model is sensitive to the choice of the magnification parameter of the photographic baseline length in images,it should be set as less than or equal to one third of the photographic baseline to ensure stable solutions.
基金supported by the National Natural Science Foundation of China under Grant No.21933006.
文摘To eliminate distortion caused by vertical drift and illusory slopes in atomic force microscopy(AFM)imaging,a lifting-wavelet-based iterative thresholding correction method is proposed in this paper.This method achieves high-quality AFM imaging via line-by-line corrections for each distorted profile along the fast axis.The key to this line-by-line correction is to accurately simulate the profile distortion of each scanning row.Therefore,a data preprocessing approach is first developed to roughly filter out most of the height data that impairs the accuracy of distortion modeling.This process is implemented through an internal double-screening mechanism.A line-fitting method is adopted to preliminarily screen out the obvious specimens.Lifting wavelet analysis is then carried out to identify the base parts that are mistakenly filtered out as specimens so as to preserve most of the base profiles and provide a good basis for further distortion modeling.Next,an iterative thresholding algorithm is developed to precisely simulate the profile distortion.By utilizing the roughly screened base profile,the optimal threshold,which is used to screen out the pure bases suitable for distortion modeling,is determined through iteration with a specified error rule.On this basis,the profile distortion is accurately modeled through line fitting on the finely screened base data,and the correction is implemented by subtracting the modeling result from the distorted profile.Finally,the effectiveness of the proposed method is verified through experiments and applications.
基金Financial support from the National Natural Science Foundation of China(grant no.U20A20154,22279005,22379006,21575016)the National Program for Support of Top-notch Young Professionals is gratefully acknowledgedtechnical support from the Xi’an Advanced Computing Center
文摘Jahn-Teller distortion(JTD)remains a fundamental bottleneck for transition metal oxides(TMOs)in electrochemical energy storage,where the e_(g)-orbital single-electron occupancy induces irreversible octahedral collapse and rapid capacity fading.Here,we pioneer an itinerant-electron-mediated dynamic suppression strategy that fundamentally reshapes the JTD evolution pathway throughπ-d orbital hybridization engineering.By constructing reduced graphene oxide/TMO heterointerfaces(rGO/MO_(x),M=Fe/Ni/Mn),localized 3d electrons are transformed into delocalized itinerant states,which(1)eliminate e_(g)-band degeneracy via orbital repopulation and(2)establish an electron density buffer layer to neutralize lattice strain.This electronic regulation enables ultrafast Na^(+)diffusion kinetics(508.3 F g^(−1)at 1 A g^(−1)→304.6 F g^(−1)at 20 A g^(−1))and near-zero lattice deformation(91.07%capacitance retention after 20,000 cycles).Synchrotron-based X-ray absorption spectroscopy and density functional theory calculations reveal that itinerant electron dynamics actively decouple the Mn^(3+)d^(4)electronic configuration from JTD triggering,leading to a dramatic suppression of octahedral distortion compared to the conventional MnO_(2).The proposed electron delocalization-to-lattice stabilization paradigm opens a universal route to design distortion-resistant electrodes for high-power energy storage systems.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12074368,92165207,12474490,12034018,and 92265113)the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0302300)+1 种基金the USTC Tang Scholarshippartially carried out at the USTC Center for Micro and Nanoscale Research and Fabrication。
文摘In semiconductor quantum dot systems,pulse distortion is a significant source of coherent errors,which impedes qubit characterization and control.Here,we demonstrate two calibration methods using a two-qubit system as the detector to correct distortion and calibrate the transfer function of the control line.Both methods are straightforward to implement,robust against noise,and applicable to a wide range of qubit types.The two methods differ in correction accuracy and complexity.The first,coarse predistortion(CPD)method,partially mitigates distortion.The second,all predistortion(APD)method,measures the transfer function and significantly enhances exchange oscillation uniformity.Both methods use exchange oscillation homogeneity as the metric and are suitable for any qubit driven by a diabatic pulse.We believe these methods will enhance qubit characterization accuracy and operation quality in future applications.
