Nano-scale chemical inhomogeneity in surface oxide films formed on a V-and N-containing martensite stainless steel and tempering heating induced changes are investigated by a combination of synchrotron-based hard X-ra...Nano-scale chemical inhomogeneity in surface oxide films formed on a V-and N-containing martensite stainless steel and tempering heating induced changes are investigated by a combination of synchrotron-based hard X-ray Photoelectron emission spectroscopy(HAXPES)and microscopy(HAXPEEM)as well as microscopic X-ray absorption spectroscopy(μ-XAS)techniques.The results reveal the inhomogeneity in the oxide films on the micron-sized Cr_(2)N-and VN-type particles,while the inhomogeneity on the martensite matrix phase exists due to localised formation of nano-sized tempering nitride particles at 600℃.The oxide film formed on Cr_(2)N-type particles is rich in Cr_(2)O_(3) compared with that on the martensite matrix and VN-type particles.With the increase of tempering temperature,Cr_(2)O_(3) formation is faster for the oxidation of Cr in the martensite matrix than the oxidation of Cr nitride-rich particles.展开更多
The infinite-layer nickelates,proposed as analogs to superconducting cuprates,provide a promising platform for exploring the mechanisms of unconventional superconductivity.However,the superconductivity has been exclus...The infinite-layer nickelates,proposed as analogs to superconducting cuprates,provide a promising platform for exploring the mechanisms of unconventional superconductivity.However,the superconductivity has been exclusively observed in thin films under atmospheric pressure,underscoring the critical role of the heterointerface.展开更多
Over the last decade,the integra-tion of scanning tunneling mi-croscopy(STM)and electron spin resonance(ESR)spectroscopy has emerged as a powerful tool for measuring spin states of surface-adsorbed molecules.The radio...Over the last decade,the integra-tion of scanning tunneling mi-croscopy(STM)and electron spin resonance(ESR)spectroscopy has emerged as a powerful tool for measuring spin states of surface-adsorbed molecules.The radio-fre-quency voltage is a key physical quantity that influences STM-ESR spectra.However,the specific effect of radio-frequency voltage on the real-time electric current associated with STM-ESR sig-nal remains unclear.In this work,we employ the hierarchical equations of motion method to simulate the STM-ESR spectra of a single spin-1/2 surface-adsorbed molecule and track the temporal evolution of the electric current,thereby elucidating how the radio-frequency volt-age influences the features of STM-ESR spectra,the real-time electric current,and the char-acteristic frequencies conveyed by the electric current.These theoretical insights facilitate a deeper comprehension of experimental phenomena.展开更多
The Savitzky-Golay(SG)filter,which employs polynomial least-squares approximations to smooth data and estimate derivatives,is widely used for processing noisy data.However,noise suppression by the SG filter is recogni...The Savitzky-Golay(SG)filter,which employs polynomial least-squares approximations to smooth data and estimate derivatives,is widely used for processing noisy data.However,noise suppression by the SG filter is recognized to be limited at data boundaries and high frequencies,which can significantly reduce the signal-to-noise ratio(SNR).To solve this problem,a novel method synergistically integrating Principal Component Analysis(PCA)with SG filtering is proposed in this paper.This approach avoids the is-sue of excessive smoothing associated with larger window sizes.The proposed PCA-SG filtering algorithm was applied to a CO gas sensing system based on Cavity Ring-Down Spectroscopy(CRDS).The perform-ance of the PCA-SG filtering algorithm is demonstrated through comparison with Moving Average Filtering(MAF),Wavelet Transformation(WT),Kalman Filtering(KF),and the SG filter.The results demonstrate that the proposed algorithm exhibits superior noise reduction capabilities compared to the other algorithms evaluated.The SNR of the ring-down signal was improved from 11.8612 dB to 29.0913 dB,and the stand-ard deviation of the extracted ring-down time constant was reduced from 0.037μs to 0.018μs.These results confirm that the proposed PCA-SG filtering algorithm effectively improves the smoothness of the ring-down curve data,demonstrating its feasibility.展开更多
Exploring cost-effective and efficient catalysts for oxygen reduction reaction(ORR)poses a significant challenge,espe-cially in the pursuit of alternatives to precious metals like platinum.Significant advancements hav...Exploring cost-effective and efficient catalysts for oxygen reduction reaction(ORR)poses a significant challenge,espe-cially in the pursuit of alternatives to precious metals like platinum.Significant advancements have driven electrochem-ists to develop efficient ORR catalysts using abundant materials,particularly iron(Fe)-based,known for their exceptional performance in ORR.While the crucial function of Fe in boosting ORR catalytic activity is recognized,the connection between material attributes and catalytic performance remains enigmatic.Understanding the dynamic processes involved in oxygen electrocatalysis is paramount for designing precious-metals-free ORR electrocatalysts.Mössbauer spectroscopy stands out as a powerful technique for deciphering the structural characteristics of Fe species in catalysis,facilitating the identification of active sites and the clarification of catalytic mechanisms.By showcasing noteworthy case studies within this review,we demonstrate the application of in-situ/operando 57Fe Mössbauer spectroscopy across diverse Fe-involved materials in ORR catalysis.This sheds light on various aspects of ORR catalysis,such as identifying active sites,assessing stability,and understanding the reaction mechanism.Our inquiry drives towards the opportunities and hurdles associ-ated with Mössbauer spectroscopy,unveiling potential breakthroughs and avenues for enhancement within this pivotal research realm.展开更多
This paper describes the design and performance of the tender energy spectroscopy beamline(BL16U1),a phase Ⅱ beamline,at the Shanghai Synchrotron Radiation Facility.The beamline,based on an in-vacuum undulator source...This paper describes the design and performance of the tender energy spectroscopy beamline(BL16U1),a phase Ⅱ beamline,at the Shanghai Synchrotron Radiation Facility.The beamline,based on an in-vacuum undulator source with 26 mm period,provides an operable energy range between 2.1 keV and 16 keV,covering the K-edges of P to Rb and L3-edges of Zr to Bi.The principal optical elements of the beamline are a toroidal mirror,a liquid nitrogen-cooled double-crystal monochromator,a high-harmonic-rejection mirror,and two pairs of Kirkpatrick–Baez(KB)mirrors.Three end-stations,including non-focusing,microprobe,and sub-microprobe types,are installed on the beamline.X-ray fluorescence(XRF)and X-ray absorption spectroscopy(XAS),including X-ray absorption near-edge structure(XANES)and extended X-ray absorption fine structure(EXAFS),are performed under vacuum or He atmosphere at the non-focusing end-station(with a beam spot size of∼670μm×710μm).Using two KB mirrors systems,micro-XRF(μXRF)mapping and micro-XANES(μXANES)studies can be performed with a spot size of approximately∼3.3μm×1.3μm at the microprobe end-station and with a smaller spot size of∼0.5μm×0.25μm at the sub-microprobe end-station.The non-focusing end-station was officially opened to users in January 2024.The microprobe and sub-microprobe end-stations will be opened to users in the near future.This paper presents the characteristics,short-term technical developments,and early experimental results of this new beamline.展开更多
Microscopy imaging is fundamental in analyzing bacterial morphology and dynamics,offering critical insights into bacterial physiology and pathogenicity.Image segmentation techniques enable quantitative analysis of bac...Microscopy imaging is fundamental in analyzing bacterial morphology and dynamics,offering critical insights into bacterial physiology and pathogenicity.Image segmentation techniques enable quantitative analysis of bacterial structures,facilitating precise measurement of morphological variations and population behaviors at single-cell resolution.This paper reviews advancements in bacterial image segmentation,emphasizing the shift from traditional thresholding and watershed methods to deep learning-driven approaches.Convolutional neural networks(CNNs),U-Net architectures,and three-dimensional(3D)frameworks excel at segmenting dense biofilms and resolving antibiotic-induced morphological changes.These methods combine automated feature extraction with physics-informed postprocessing.Despite progress,challenges persist in computational efficiency,cross-species generalizability,and integration with multimodal experimental workflows.Future progress will depend on improving model robustness across species and imaging modalities,integrating multimodal data for phenotype-function mapping,and developing standard pipelines that link computational tools with clinical diagnostics.These innovations will expand microbial phenotyping beyond structural analysis,enabling deeper insights into bacterial physiology and ecological interactions.展开更多
Desulfurization of CaO–Al_(2)O_(3) particles in molten steel was observed in situ using high-temperature confocal scanning laser microscopy.The effects of the aluminum and silicon contents of molten steel on desulfur...Desulfurization of CaO–Al_(2)O_(3) particles in molten steel was observed in situ using high-temperature confocal scanning laser microscopy.The effects of the aluminum and silicon contents of molten steel on desulfurization were analyzed.When the total aluminum content in the steel increased from 6 to 1100 ppm,the CaS content in CaO–Al_(2)O_(3) particles increased from 2.1wt%to 84.84wt%after the reaction for 90 s.Furthermore,when the silicon content in the steel increased from 0.01wt%to 2.20wt%,the CaS content in CaO–Al_(2)O_(3) particles increased from 1.53wt%to 79.01wt%after the reaction for 90 s.This indicates that the increase in the aluminum and silicon contents of the steel promoted the desulfurization of CaO–Al_(2)O_(3) particles.A kinetic model was established to predict the CaO–Al_(2)O_(3) particles composition,and the diffusion coefficient of sulfur in CaO–Al_(2)O_(3) particles was 9.375×10^(−10)m^(2)·s^(−1) at 1600℃,which provided a new method for the calculation of diffusion coefficient.展开更多
The formation of copper deposits is closely related to hydrothermal processes.Understanding the migration of copper in hydrothermal fluids aids in reconstructing mineralization processes and deciphering deposit genesi...The formation of copper deposits is closely related to hydrothermal processes.Understanding the migration of copper in hydrothermal fluids aids in reconstructing mineralization processes and deciphering deposit genesis.Copper primarily exists as Cu^(+)and Cu^(2+)in hydrothermal solutions,with redox conditions governing their interconversion.In chloride-rich geological fluids,Cu-Cl complexes are considered critical for copper transport.However,the specific types and valence transitions of Cu-Cl complexes under varying hydrothermal conditions remain poorly understood.This study employed in situ Raman spectroscopy to systematically analyze Cu+HCl and CuCl_(2)+K_(2)S_(2)O_(3)/H_(2) systems under saturated vapor pressure at 25-300℃,elucidating the effects of temperature,Cl^(-)concentration,and redox conditions on copper speciation.In the Cu^(+)HCl system,copper dissolved as monovalent Cu-Cl complexes.At high temperatures(>200℃),[CuCl_(2)]^(-)is the dominated species,whereas[CuCl_(3)]^(2-)becomes prevalent at lower temperatures and higher HCl concentrations.For the Cu^(2+)-Cl system,the dominant species transitioned from[Cu(H_(2)O)n]^(2+)(<50℃)to[CuCl_(4)]^(2-)(100℃)and further to[CuCl]^(+)and[CuCl_(2)]^(0) at 300℃.The introduction of reducing agents(K_(2)S_(2)O_(3)/H_(2))facilitated Cu^(2+)→Cu^(+)reduction,thereby stabilizing Cu^(+)-Cl complexes and inducing partial copper precipitation.The behavior of copper in chloriderich hydrothermal fluids observed in this study indicates that high-temperature oxidizing fluids facilitate Cu mobilization,while cooling and redox changes promote deposition and ore minerals formation.展开更多
The spatially-resolved laser-based high resolution angle resolved photoemission spectroscopy(ARPES)measurements have been performed on the optimally-doped HgBa_(2)Ca_(2)Cu_(3)O_(8+δ)(Hg1223)superconductor with a T_(c...The spatially-resolved laser-based high resolution angle resolved photoemission spectroscopy(ARPES)measurements have been performed on the optimally-doped HgBa_(2)Ca_(2)Cu_(3)O_(8+δ)(Hg1223)superconductor with a T_(c) of 133 K.Two distinct regions are identified on the cleaved surface:the single Fermi surface region where only one Fermi surface is observed,and the double Fermi surface region where two Fermi surface sheets are resolved coming from both the inner(IP)and outer(OP)CuO_(2) planes.The electronic structure and superconducting gap are measured on both of these two regions.In both cases,the observed electronic states are mainly concentrated near the nodal region.The momentum dependence of the superconducting gap deviates from the standard d-wave form.These results indicate that the surface electronic structure of Hg1223 behaves more like that of underdoped cuprates.展开更多
[Objectives]This study was conducted to achieve rapid and accurate detection of protein content in rice with a particle size of 1.0 mm.[Methods]A multi-model fusion strategy was proposed on the basis of Stacking ensem...[Objectives]This study was conducted to achieve rapid and accurate detection of protein content in rice with a particle size of 1.0 mm.[Methods]A multi-model fusion strategy was proposed on the basis of Stacking ensemble learning.A base learner pool was constructed,containing Partial Least Squares(PLS),Support Vector Machine(SVM),Deep Extreme Learning Machine(DELM),Random Forest(RF),Gradient Boosting Decision Tree(GBDT),and Multilayer Perceptron(MLP).PLS,DELM,and Linear Regression(LR)were used as meta-learner candidates.Employing integer coding technology,systematic dynamic combinations of base learners and meta-learners were generated,resulting in a total of 40 non-repetitive fusion models.The optimal combination was selected through a comprehensive evaluation based on multiple assessment indicators.[Results]The combination"PLS-DELM-MLP-LR"(code 1367)achieved coefficients of determination of 0.9732 and 0.9780 on the validation set and independent test set,respectively,with relative root mean square errors of 2.35%and 2.36%,and residual predictive deviations of 6.1075 and 6.7479,respectively.[Conclusions]The Stacking fusion model significantly enhances the predictive accuracy and robustness of spectral quantitative analysis,providing an efficient and feasible solution for modeling complex agricultural product spectral data.展开更多
A RadioFrequency Quadrupole(RFQ)cooler-buncher system was developed and implemented in a collinear laser spectroscopy setup.This system converts a continuous ion beam into short bunches while enhancing the beam qualit...A RadioFrequency Quadrupole(RFQ)cooler-buncher system was developed and implemented in a collinear laser spectroscopy setup.This system converts a continuous ion beam into short bunches while enhancing the beam quality and reducing the energy spread.The functionality of the RFQ cooler buncher was verified through offline tests with stable rubidium and indium beams delivered from a surface ion source and a laser ablation ion source,respectively.Bunched ion beams with a full width at half maximum of approximately 2μs in the time-of-flight spectrum were successfully achieved with a transmission efficiency exceeding 60%.The implementation of the RFQ cooler-buncher system also significantly improved the overall transmission efficiency of the collinear laser spectroscopy setup.展开更多
The pseudo-two-dimensional(P2D)model plays an important role in exploring physicochemical mechanisms,predicting the state of health,and improving the fast charge capability for Li-ion batteries(LIBs).However,the fast ...The pseudo-two-dimensional(P2D)model plays an important role in exploring physicochemical mechanisms,predicting the state of health,and improving the fast charge capability for Li-ion batteries(LIBs).However,the fast charge leads to the lithium concentration gradient in the solid and electrolyte phases and the non-uniform electrochemical reaction at the solid/electrolyte interface.In order to decouple charge transfer reactions in LIBs under dynamic conditions,understanding the spatio-temporal resolution of the P2D model is urgently required.Till now,the study of this aspect is still insufficient.This work studies the spatio-temporal resolution for dynamic/static electrochemical impedance spectroscopy(DEIS/SEIS)on multiple scales.In detail,DEIS and SEIS with spatio-temporal resolutions are used to decouple charge transfer reactions in LIBs based on the numerical solution of the P2D model in the frequency domain.The calculated results indicate that decoupling solid diffusion requires a high spatial resolution along the r-direction in particles,decoupling electrolyte diffusion and interfacial transfer reaction requires a high spatial resolution along the x-direction,and decoupling charge transfer reactions in LIBs at an extremely low state of charge(SOC)requires an extremely high temporal resolution along the t-direction.Finally,the optimal range of spatio-temporal resolutions for DEIS/SEIS is derived,and the method to decouple charge transfer reactions with spatio-temporal resolutions is developed.展开更多
This study investigated the heterogeneous responses of organic matter(OM)in highly-to over-mature source rocks during thermal maturation.An integrated analysis was conducted on the Raman spectroscopic and geochemical ...This study investigated the heterogeneous responses of organic matter(OM)in highly-to over-mature source rocks during thermal maturation.An integrated analysis was conducted on the Raman spectroscopic and geochemical signatures of shales from the Lower Silurian Longmaxi Formation and the Lower Cambrian Qiongzhusi Formation,as well as anthracites from the Lower Permian Shanxi–Formation and the Upper Carboniferous Taiyuan Formation(collectively referred to as the Shanxi Taiyuan Formations).Additionally,burial and thermal evolution modeling was employed to support the analysis.A systematic assessment of Raman spectral parameters(e.g.,the positions and intensity ratio of the D and G bands)revealed robust correlations between the thermal history patterns of source rocks and molecular structural evolution parameters.The subsequent mechanistic quantification demonstrated that the maturation state of the source rocks was subjected to the hierarchical control of three principal factors:Peak heating temperature,the duration of sustained thermal intensity,and effective maturation duration.In addition,comparative analyses demonstrated that the anthracites attained higher structural ordering under sustained thermal conditions.This contrasts with the disordered carbon matrices observed in the intermittently heated shales.Raman spectroscopy further revealed broader variations in the D and G band intensities of the Longmaxi Formation compared to the Qiongzhusi Formation.This difference is associated with their different thermal histories.The thermal burial histories confirm that shales in the Longmaxi Formation underwent thermal exposure at lower peak temperatures over a shorter duration compared to those in the Qiongzhusi Formation.Finally,this study established a maturity calibration model for over-mature source rocks through a systematic correlation between Raman peak height ratios(R_(D/G))and vitrinite reflectance(R_(o)).展开更多
Many spore-forming Bacillus species can cause serious human diseases,because of accidental Bacillusspore infection.Thus,developing an identification strategy with both high sensitivity and specificity is greatly in de...Many spore-forming Bacillus species can cause serious human diseases,because of accidental Bacillusspore infection.Thus,developing an identification strategy with both high sensitivity and specificity is greatly in demand.In this work,we proposed a novel approach named multi-head self-attention mechanism-guided neural network Raman platform to identify living Bacillus spores within a single-cell resolution.The multi-head self-attention mechanism-guided neural network Raman platform was created by combining single-cell Raman spectroscopy,convolutional neural network(CNN),and multi-head self-attention mechanism.To address the limited size of the original spectra dataset,Gaussian noise-based spectra augmentation was employed to increase the number of single-cell Raman spectra datasets for CNN training.Owing to the assistance of both spectra augmentation and multi-head self-attention mechanism,the obtained prediction accuracy of five Bacillus spore species was further improved from 92.29±0.82%to 99.43±0.15%.To figure out the spectra differences covered by the multi-head self-attention mechanism-guided CNN,the relative classification weight from typical Raman bands was visualized via multi-head self-attention mechanism curve.In the process of spectra augmentation from 0 to 1000,the distribution of relative classification weight varied from a discrete state to a more concentrated phase.More importantly,these highlighted four Raman bands(1017,1449,1576,and 1660 cm^(-1))were assigned large weights,showing that the spectra differences in the Raman bands produced the largest contribution to prediction accuracy.It can be foreseen that,our proposed sorting platform has great potential in accurately identifying Bacillus and its related genera species at a single-cell level.展开更多
The assembling behavior and electronic properties of asymmetric tris(phthalocyaninato)lutetium triple-decker sandwich complex molecules(Lu2Pc3)on highly oriented pyrolytic graphite(HOPG)surfaces have been studied by s...The assembling behavior and electronic properties of asymmetric tris(phthalocyaninato)lutetium triple-decker sandwich complex molecules(Lu2Pc3)on highly oriented pyrolytic graphite(HOPG)surfaces have been studied by scanning tunneling microscopy/spectroscopy(STM/STS)methods.Phase transitions were observed at different bias polarities,involving an ordered packing arrangement with fourfold symmetry at negative bias and an amorphous arrangement at positive bias.Molecular switching behaviour for individual Lu2Pc3 molecules was reported here according to the bias-polarity-induced flipping phenomena and the peak shift in dI/dV versus V curves at different voltage scanning directions.The sensitive response of the strong intrinsic molecular dipole to an external electric field is proposed to be responsible for molecular switching of Lu_(2)Pc_(3)at the solid/liquid interface.展开更多
Scanning tunneling microscopy/spectroscopy(STM/STS)at 4.8 K has been used to examine the growth of a double-decker bis(phthalocyaninato)yttrium(YP_(c2))molecule on a reconstructed Au(111)substrate.Local differential c...Scanning tunneling microscopy/spectroscopy(STM/STS)at 4.8 K has been used to examine the growth of a double-decker bis(phthalocyaninato)yttrium(YP_(c2))molecule on a reconstructed Au(111)substrate.Local differential conductance spectra(dI/dV)of a single YPc2 molecule allow the characteristics of the highest occupied molecular orbital(HOMO)and the lowest unoccupied molecular orbital(LUMO)to be identified.Furthermore,lateral distributions of the local density of states(LDOS)have also been obtained by dI/dV mapping and confirmed by first principles simulations.These electronic feature mappings and theoretical calculations provide a basis for understanding the unique STM morphology of YPc2,which is usually imaged as an eight-lobed structure.In addition,we demonstrate that bias-dependent STM morphologies and simultaneous dI/dV maps can provide a way of understanding the stability of two-dimensional YP_(c2) films.展开更多
By Using （scanning） transmission electron microscopy, localized-corrosion morphology variations of the AA7055 AIZn（Cu）Mg alloy with different thermal processes and their underlying microscopic causes were investig...By Using （scanning） transmission electron microscopy, localized-corrosion morphology variations of the AA7055 AIZn（Cu）Mg alloy with different thermal processes and their underlying microscopic causes were investigated systematically. Our study shows that the corrosion resistance of the nanoscale precipitates varies with their structure type and Cu-content. Just like the Al-matrix, the early-stage precipitates are corrosion resistant, as compared with the ηp/η-precipitates without high Cu-content. With a high Cu-content, however, the η-precipitates become most corrosion resistant among all phases involved. Hence, tailoring the precipitate microstructure and chemistry though thermal processes may change the overall corrosion morphology and improve corrosion resistance property of the alloy.展开更多
Through the investigation of the sample surface and interface of 3, 4, 9, 10-perylenetetracarboxylic dianhydride （PTCDA）/indium-tin-oxide （ITO） thin films using atomic force microscopy, it has been found that the ...Through the investigation of the sample surface and interface of 3, 4, 9, 10-perylenetetracarboxylic dianhydride （PTCDA）/indium-tin-oxide （ITO） thin films using atomic force microscopy, it has been found that the surface is complanate, the growth is uniform and the defects cover basically the surface of ITO. Furthermore, the number of pinholes is small. The analysis of the sample surface and interface further verifies this result by using x-ray photoemission spectroscopy. At the same time, PTCDA is found to have the ability of restraining the diffusion of chemical constituents from ITO to the hole transport layer, which is beneficial to the improvement of the performance and the useful lifetime of the organic light emitting diodes （OLEDs）.展开更多
基金supported by the Vinnova(project number 2020-03778)supported by the Swedish Research Council(Vetenskapsradet,project number 2021-04157).
文摘Nano-scale chemical inhomogeneity in surface oxide films formed on a V-and N-containing martensite stainless steel and tempering heating induced changes are investigated by a combination of synchrotron-based hard X-ray Photoelectron emission spectroscopy(HAXPES)and microscopy(HAXPEEM)as well as microscopic X-ray absorption spectroscopy(μ-XAS)techniques.The results reveal the inhomogeneity in the oxide films on the micron-sized Cr_(2)N-and VN-type particles,while the inhomogeneity on the martensite matrix phase exists due to localised formation of nano-sized tempering nitride particles at 600℃.The oxide film formed on Cr_(2)N-type particles is rich in Cr_(2)O_(3) compared with that on the martensite matrix and VN-type particles.With the increase of tempering temperature,Cr_(2)O_(3) formation is faster for the oxidation of Cr in the martensite matrix than the oxidation of Cr nitride-rich particles.
基金supported by the National Natural Science Foundation of China[52125307(to P.G.),12404192(to R.C.S),12274061(to L.Q.)]Key Research and Development Program from the Ministry of Science and Technology(2023YFA1406301)the support from the New Cornerstone Science Foundation through the XPLORER PRIZE。
文摘The infinite-layer nickelates,proposed as analogs to superconducting cuprates,provide a promising platform for exploring the mechanisms of unconventional superconductivity.However,the superconductivity has been exclusively observed in thin films under atmospheric pressure,underscoring the critical role of the heterointerface.
基金supported by the National Natural Sci-ence Foundation of China(Nos.22203083,22425301,22393912)Strategic Priority Research Pro-gram of the Chinese Academy of Sciences(No.XDB0450101).
文摘Over the last decade,the integra-tion of scanning tunneling mi-croscopy(STM)and electron spin resonance(ESR)spectroscopy has emerged as a powerful tool for measuring spin states of surface-adsorbed molecules.The radio-fre-quency voltage is a key physical quantity that influences STM-ESR spectra.However,the specific effect of radio-frequency voltage on the real-time electric current associated with STM-ESR sig-nal remains unclear.In this work,we employ the hierarchical equations of motion method to simulate the STM-ESR spectra of a single spin-1/2 surface-adsorbed molecule and track the temporal evolution of the electric current,thereby elucidating how the radio-frequency volt-age influences the features of STM-ESR spectra,the real-time electric current,and the char-acteristic frequencies conveyed by the electric current.These theoretical insights facilitate a deeper comprehension of experimental phenomena.
文摘The Savitzky-Golay(SG)filter,which employs polynomial least-squares approximations to smooth data and estimate derivatives,is widely used for processing noisy data.However,noise suppression by the SG filter is recognized to be limited at data boundaries and high frequencies,which can significantly reduce the signal-to-noise ratio(SNR).To solve this problem,a novel method synergistically integrating Principal Component Analysis(PCA)with SG filtering is proposed in this paper.This approach avoids the is-sue of excessive smoothing associated with larger window sizes.The proposed PCA-SG filtering algorithm was applied to a CO gas sensing system based on Cavity Ring-Down Spectroscopy(CRDS).The perform-ance of the PCA-SG filtering algorithm is demonstrated through comparison with Moving Average Filtering(MAF),Wavelet Transformation(WT),Kalman Filtering(KF),and the SG filter.The results demonstrate that the proposed algorithm exhibits superior noise reduction capabilities compared to the other algorithms evaluated.The SNR of the ring-down signal was improved from 11.8612 dB to 29.0913 dB,and the stand-ard deviation of the extracted ring-down time constant was reduced from 0.037μs to 0.018μs.These results confirm that the proposed PCA-SG filtering algorithm effectively improves the smoothness of the ring-down curve data,demonstrating its feasibility.
基金financially supported by the National Natural Science Foundation of China (22350410386,W2412116,22375200,U22A202175,21961142006)。
文摘Exploring cost-effective and efficient catalysts for oxygen reduction reaction(ORR)poses a significant challenge,espe-cially in the pursuit of alternatives to precious metals like platinum.Significant advancements have driven electrochem-ists to develop efficient ORR catalysts using abundant materials,particularly iron(Fe)-based,known for their exceptional performance in ORR.While the crucial function of Fe in boosting ORR catalytic activity is recognized,the connection between material attributes and catalytic performance remains enigmatic.Understanding the dynamic processes involved in oxygen electrocatalysis is paramount for designing precious-metals-free ORR electrocatalysts.Mössbauer spectroscopy stands out as a powerful technique for deciphering the structural characteristics of Fe species in catalysis,facilitating the identification of active sites and the clarification of catalytic mechanisms.By showcasing noteworthy case studies within this review,we demonstrate the application of in-situ/operando 57Fe Mössbauer spectroscopy across diverse Fe-involved materials in ORR catalysis.This sheds light on various aspects of ORR catalysis,such as identifying active sites,assessing stability,and understanding the reaction mechanism.Our inquiry drives towards the opportunities and hurdles associ-ated with Mössbauer spectroscopy,unveiling potential breakthroughs and avenues for enhancement within this pivotal research realm.
基金supported by the National Key R&D Program of China(No.2021YFA1601003)the financial support of the SSRF PhaseⅡproject.
文摘This paper describes the design and performance of the tender energy spectroscopy beamline(BL16U1),a phase Ⅱ beamline,at the Shanghai Synchrotron Radiation Facility.The beamline,based on an in-vacuum undulator source with 26 mm period,provides an operable energy range between 2.1 keV and 16 keV,covering the K-edges of P to Rb and L3-edges of Zr to Bi.The principal optical elements of the beamline are a toroidal mirror,a liquid nitrogen-cooled double-crystal monochromator,a high-harmonic-rejection mirror,and two pairs of Kirkpatrick–Baez(KB)mirrors.Three end-stations,including non-focusing,microprobe,and sub-microprobe types,are installed on the beamline.X-ray fluorescence(XRF)and X-ray absorption spectroscopy(XAS),including X-ray absorption near-edge structure(XANES)and extended X-ray absorption fine structure(EXAFS),are performed under vacuum or He atmosphere at the non-focusing end-station(with a beam spot size of∼670μm×710μm).Using two KB mirrors systems,micro-XRF(μXRF)mapping and micro-XANES(μXANES)studies can be performed with a spot size of approximately∼3.3μm×1.3μm at the microprobe end-station and with a smaller spot size of∼0.5μm×0.25μm at the sub-microprobe end-station.The non-focusing end-station was officially opened to users in January 2024.The microprobe and sub-microprobe end-stations will be opened to users in the near future.This paper presents the characteristics,short-term technical developments,and early experimental results of this new beamline.
基金financially supported by the Open Project Program of Wuhan National Laboratory for Optoelectronics(No.2022WNLOKF009)the National Natural Science Foundation of China(No.62475216)+2 种基金the Key Research and Development Program of Shaanxi(No.2024GH-ZDXM-37)the Fujian Provincial Natural Science Foundation of China(No.2024J01060)the Startup Program of XMU,and the Fundamental Research Funds for the Central Universities.
文摘Microscopy imaging is fundamental in analyzing bacterial morphology and dynamics,offering critical insights into bacterial physiology and pathogenicity.Image segmentation techniques enable quantitative analysis of bacterial structures,facilitating precise measurement of morphological variations and population behaviors at single-cell resolution.This paper reviews advancements in bacterial image segmentation,emphasizing the shift from traditional thresholding and watershed methods to deep learning-driven approaches.Convolutional neural networks(CNNs),U-Net architectures,and three-dimensional(3D)frameworks excel at segmenting dense biofilms and resolving antibiotic-induced morphological changes.These methods combine automated feature extraction with physics-informed postprocessing.Despite progress,challenges persist in computational efficiency,cross-species generalizability,and integration with multimodal experimental workflows.Future progress will depend on improving model robustness across species and imaging modalities,integrating multimodal data for phenotype-function mapping,and developing standard pipelines that link computational tools with clinical diagnostics.These innovations will expand microbial phenotyping beyond structural analysis,enabling deeper insights into bacterial physiology and ecological interactions.
基金supported by the National Key R&D Program of China(No.2023YFB3709900)the National Nature Science Foundation of China(No.U22A20171)+1 种基金the China Baowu Low Carbon Metallurgy Innovation Foundation(No.BWLCF202315)the High Steel Center(HSC)at North China University of Technology and University of Science and Technology Beijing,China.
文摘Desulfurization of CaO–Al_(2)O_(3) particles in molten steel was observed in situ using high-temperature confocal scanning laser microscopy.The effects of the aluminum and silicon contents of molten steel on desulfurization were analyzed.When the total aluminum content in the steel increased from 6 to 1100 ppm,the CaS content in CaO–Al_(2)O_(3) particles increased from 2.1wt%to 84.84wt%after the reaction for 90 s.Furthermore,when the silicon content in the steel increased from 0.01wt%to 2.20wt%,the CaS content in CaO–Al_(2)O_(3) particles increased from 1.53wt%to 79.01wt%after the reaction for 90 s.This indicates that the increase in the aluminum and silicon contents of the steel promoted the desulfurization of CaO–Al_(2)O_(3) particles.A kinetic model was established to predict the CaO–Al_(2)O_(3) particles composition,and the diffusion coefficient of sulfur in CaO–Al_(2)O_(3) particles was 9.375×10^(−10)m^(2)·s^(−1) at 1600℃,which provided a new method for the calculation of diffusion coefficient.
基金jointly funded by the Strategic Priority Research Program of the Chinese Academy of Sciences(grant No.XDA0430301)the National Natural Science Foundation of China(grant Nos.42130109,41973059)。
文摘The formation of copper deposits is closely related to hydrothermal processes.Understanding the migration of copper in hydrothermal fluids aids in reconstructing mineralization processes and deciphering deposit genesis.Copper primarily exists as Cu^(+)and Cu^(2+)in hydrothermal solutions,with redox conditions governing their interconversion.In chloride-rich geological fluids,Cu-Cl complexes are considered critical for copper transport.However,the specific types and valence transitions of Cu-Cl complexes under varying hydrothermal conditions remain poorly understood.This study employed in situ Raman spectroscopy to systematically analyze Cu+HCl and CuCl_(2)+K_(2)S_(2)O_(3)/H_(2) systems under saturated vapor pressure at 25-300℃,elucidating the effects of temperature,Cl^(-)concentration,and redox conditions on copper speciation.In the Cu^(+)HCl system,copper dissolved as monovalent Cu-Cl complexes.At high temperatures(>200℃),[CuCl_(2)]^(-)is the dominated species,whereas[CuCl_(3)]^(2-)becomes prevalent at lower temperatures and higher HCl concentrations.For the Cu^(2+)-Cl system,the dominant species transitioned from[Cu(H_(2)O)n]^(2+)(<50℃)to[CuCl_(4)]^(2-)(100℃)and further to[CuCl]^(+)and[CuCl_(2)]^(0) at 300℃.The introduction of reducing agents(K_(2)S_(2)O_(3)/H_(2))facilitated Cu^(2+)→Cu^(+)reduction,thereby stabilizing Cu^(+)-Cl complexes and inducing partial copper precipitation.The behavior of copper in chloriderich hydrothermal fluids observed in this study indicates that high-temperature oxidizing fluids facilitate Cu mobilization,while cooling and redox changes promote deposition and ore minerals formation.
基金supported by the National Key Research and Development Program of China(Grant Nos.2021YFA1401800,2022YFA1604200,2022YFA1403900,2023YFA1406002,2024YFA1408301 and 2024YFA1408100)the National Natural Science Foun-dation of China(Grant Nos.12488201,12374066,12374154,12494593)+2 种基金Quantum Science and Technology-National Science and Technology Major Project(Grant No.2021ZD0301800)CAS Superconducting Research Project(Grant No.SCZX-0101)the Synergetic Extreme Condition User Facility(SECUF).
文摘The spatially-resolved laser-based high resolution angle resolved photoemission spectroscopy(ARPES)measurements have been performed on the optimally-doped HgBa_(2)Ca_(2)Cu_(3)O_(8+δ)(Hg1223)superconductor with a T_(c) of 133 K.Two distinct regions are identified on the cleaved surface:the single Fermi surface region where only one Fermi surface is observed,and the double Fermi surface region where two Fermi surface sheets are resolved coming from both the inner(IP)and outer(OP)CuO_(2) planes.The electronic structure and superconducting gap are measured on both of these two regions.In both cases,the observed electronic states are mainly concentrated near the nodal region.The momentum dependence of the superconducting gap deviates from the standard d-wave form.These results indicate that the surface electronic structure of Hg1223 behaves more like that of underdoped cuprates.
文摘[Objectives]This study was conducted to achieve rapid and accurate detection of protein content in rice with a particle size of 1.0 mm.[Methods]A multi-model fusion strategy was proposed on the basis of Stacking ensemble learning.A base learner pool was constructed,containing Partial Least Squares(PLS),Support Vector Machine(SVM),Deep Extreme Learning Machine(DELM),Random Forest(RF),Gradient Boosting Decision Tree(GBDT),and Multilayer Perceptron(MLP).PLS,DELM,and Linear Regression(LR)were used as meta-learner candidates.Employing integer coding technology,systematic dynamic combinations of base learners and meta-learners were generated,resulting in a total of 40 non-repetitive fusion models.The optimal combination was selected through a comprehensive evaluation based on multiple assessment indicators.[Results]The combination"PLS-DELM-MLP-LR"(code 1367)achieved coefficients of determination of 0.9732 and 0.9780 on the validation set and independent test set,respectively,with relative root mean square errors of 2.35%and 2.36%,and residual predictive deviations of 6.1075 and 6.7479,respectively.[Conclusions]The Stacking fusion model significantly enhances the predictive accuracy and robustness of spectral quantitative analysis,providing an efficient and feasible solution for modeling complex agricultural product spectral data.
基金supported by the National Natural Science Foundation of China(Nos.12027809,12350007)National Key R&D Program of China(Nos.2022YFA1605100,2023YFA1606403,and 2023YFE0101600)+1 种基金New Cornerstone Science Foundation through the XPLORER PRIZEfunding from the European Research Council(ERC)under the European Union’s Horizon 2020 research and innovation program under grant agreement No.679038.
文摘A RadioFrequency Quadrupole(RFQ)cooler-buncher system was developed and implemented in a collinear laser spectroscopy setup.This system converts a continuous ion beam into short bunches while enhancing the beam quality and reducing the energy spread.The functionality of the RFQ cooler buncher was verified through offline tests with stable rubidium and indium beams delivered from a surface ion source and a laser ablation ion source,respectively.Bunched ion beams with a full width at half maximum of approximately 2μs in the time-of-flight spectrum were successfully achieved with a transmission efficiency exceeding 60%.The implementation of the RFQ cooler-buncher system also significantly improved the overall transmission efficiency of the collinear laser spectroscopy setup.
基金supported by the National Natural Science Foundation of China(Nos.22479092 and 22078190)。
文摘The pseudo-two-dimensional(P2D)model plays an important role in exploring physicochemical mechanisms,predicting the state of health,and improving the fast charge capability for Li-ion batteries(LIBs).However,the fast charge leads to the lithium concentration gradient in the solid and electrolyte phases and the non-uniform electrochemical reaction at the solid/electrolyte interface.In order to decouple charge transfer reactions in LIBs under dynamic conditions,understanding the spatio-temporal resolution of the P2D model is urgently required.Till now,the study of this aspect is still insufficient.This work studies the spatio-temporal resolution for dynamic/static electrochemical impedance spectroscopy(DEIS/SEIS)on multiple scales.In detail,DEIS and SEIS with spatio-temporal resolutions are used to decouple charge transfer reactions in LIBs based on the numerical solution of the P2D model in the frequency domain.The calculated results indicate that decoupling solid diffusion requires a high spatial resolution along the r-direction in particles,decoupling electrolyte diffusion and interfacial transfer reaction requires a high spatial resolution along the x-direction,and decoupling charge transfer reactions in LIBs at an extremely low state of charge(SOC)requires an extremely high temporal resolution along the t-direction.Finally,the optimal range of spatio-temporal resolutions for DEIS/SEIS is derived,and the method to decouple charge transfer reactions with spatio-temporal resolutions is developed.
基金supported by the National Natural Science Foundation of China(42362022)the Open Fund of the Shaanxi Key Laboratory of Petroleum Accumulation Geology(PAG-202406)the Open Fund of the Mine Geology and Environment Academician and Expert Workstation(2024OITYSZJGZZ-005)。
文摘This study investigated the heterogeneous responses of organic matter(OM)in highly-to over-mature source rocks during thermal maturation.An integrated analysis was conducted on the Raman spectroscopic and geochemical signatures of shales from the Lower Silurian Longmaxi Formation and the Lower Cambrian Qiongzhusi Formation,as well as anthracites from the Lower Permian Shanxi–Formation and the Upper Carboniferous Taiyuan Formation(collectively referred to as the Shanxi Taiyuan Formations).Additionally,burial and thermal evolution modeling was employed to support the analysis.A systematic assessment of Raman spectral parameters(e.g.,the positions and intensity ratio of the D and G bands)revealed robust correlations between the thermal history patterns of source rocks and molecular structural evolution parameters.The subsequent mechanistic quantification demonstrated that the maturation state of the source rocks was subjected to the hierarchical control of three principal factors:Peak heating temperature,the duration of sustained thermal intensity,and effective maturation duration.In addition,comparative analyses demonstrated that the anthracites attained higher structural ordering under sustained thermal conditions.This contrasts with the disordered carbon matrices observed in the intermittently heated shales.Raman spectroscopy further revealed broader variations in the D and G band intensities of the Longmaxi Formation compared to the Qiongzhusi Formation.This difference is associated with their different thermal histories.The thermal burial histories confirm that shales in the Longmaxi Formation underwent thermal exposure at lower peak temperatures over a shorter duration compared to those in the Qiongzhusi Formation.Finally,this study established a maturity calibration model for over-mature source rocks through a systematic correlation between Raman peak height ratios(R_(D/G))and vitrinite reflectance(R_(o)).
基金partially supported by the National Natural Science Foundation of China(62075137)the Guangdong Basic and Applied Basic Research Foundation(2023A1515140161)+3 种基金the Guangxi Natural Science Foundation of China(2021JJB 110003)the Dongguan Science and Technology of Social Development Program(20231800936312)the high-level talent program of Dongguan University of Technology(No.221110080)the Sanming Project of Medicine in Shenzhen(No.SZSM202103014).
文摘Many spore-forming Bacillus species can cause serious human diseases,because of accidental Bacillusspore infection.Thus,developing an identification strategy with both high sensitivity and specificity is greatly in demand.In this work,we proposed a novel approach named multi-head self-attention mechanism-guided neural network Raman platform to identify living Bacillus spores within a single-cell resolution.The multi-head self-attention mechanism-guided neural network Raman platform was created by combining single-cell Raman spectroscopy,convolutional neural network(CNN),and multi-head self-attention mechanism.To address the limited size of the original spectra dataset,Gaussian noise-based spectra augmentation was employed to increase the number of single-cell Raman spectra datasets for CNN training.Owing to the assistance of both spectra augmentation and multi-head self-attention mechanism,the obtained prediction accuracy of five Bacillus spore species was further improved from 92.29±0.82%to 99.43±0.15%.To figure out the spectra differences covered by the multi-head self-attention mechanism-guided CNN,the relative classification weight from typical Raman bands was visualized via multi-head self-attention mechanism curve.In the process of spectra augmentation from 0 to 1000,the distribution of relative classification weight varied from a discrete state to a more concentrated phase.More importantly,these highlighted four Raman bands(1017,1449,1576,and 1660 cm^(-1))were assigned large weights,showing that the spectra differences in the Raman bands produced the largest contribution to prediction accuracy.It can be foreseen that,our proposed sorting platform has great potential in accurately identifying Bacillus and its related genera species at a single-cell level.
基金the National Natural Science Foundation of China(90406019,20573116,and 20673029)the National Basic Research Program of China(973 Program,2006CB932100).
文摘The assembling behavior and electronic properties of asymmetric tris(phthalocyaninato)lutetium triple-decker sandwich complex molecules(Lu2Pc3)on highly oriented pyrolytic graphite(HOPG)surfaces have been studied by scanning tunneling microscopy/spectroscopy(STM/STS)methods.Phase transitions were observed at different bias polarities,involving an ordered packing arrangement with fourfold symmetry at negative bias and an amorphous arrangement at positive bias.Molecular switching behaviour for individual Lu2Pc3 molecules was reported here according to the bias-polarity-induced flipping phenomena and the peak shift in dI/dV versus V curves at different voltage scanning directions.The sensitive response of the strong intrinsic molecular dipole to an external electric field is proposed to be responsible for molecular switching of Lu_(2)Pc_(3)at the solid/liquid interface.
基金The first author acknowledges the financial support of JSPS(Japan Society for the Promotion of Science)This work was also supported by an International Colla-borative Research Grant by the National Institute of Information and Communications Technology of Japan.
文摘Scanning tunneling microscopy/spectroscopy(STM/STS)at 4.8 K has been used to examine the growth of a double-decker bis(phthalocyaninato)yttrium(YP_(c2))molecule on a reconstructed Au(111)substrate.Local differential conductance spectra(dI/dV)of a single YPc2 molecule allow the characteristics of the highest occupied molecular orbital(HOMO)and the lowest unoccupied molecular orbital(LUMO)to be identified.Furthermore,lateral distributions of the local density of states(LDOS)have also been obtained by dI/dV mapping and confirmed by first principles simulations.These electronic feature mappings and theoretical calculations provide a basis for understanding the unique STM morphology of YPc2,which is usually imaged as an eight-lobed structure.In addition,we demonstrate that bias-dependent STM morphologies and simultaneous dI/dV maps can provide a way of understanding the stability of two-dimensional YP_(c2) films.
基金financially supported by the National Natural Science Foundation of China(Nos.51501059,51471067,51501060,and 11427806)the National Key Research and Development Program of China(No.2016YFB0300801)
文摘By Using （scanning） transmission electron microscopy, localized-corrosion morphology variations of the AA7055 AIZn（Cu）Mg alloy with different thermal processes and their underlying microscopic causes were investigated systematically. Our study shows that the corrosion resistance of the nanoscale precipitates varies with their structure type and Cu-content. Just like the Al-matrix, the early-stage precipitates are corrosion resistant, as compared with the ηp/η-precipitates without high Cu-content. With a high Cu-content, however, the η-precipitates become most corrosion resistant among all phases involved. Hence, tailoring the precipitate microstructure and chemistry though thermal processes may change the overall corrosion morphology and improve corrosion resistance property of the alloy.
基金Project supported by the National Natural Science Foundation of China （Grant No 60276026） and the Natural Science Foundation of Gansu Province, China （Grant No ZS031-A25-012-G）.
文摘Through the investigation of the sample surface and interface of 3, 4, 9, 10-perylenetetracarboxylic dianhydride （PTCDA）/indium-tin-oxide （ITO） thin films using atomic force microscopy, it has been found that the surface is complanate, the growth is uniform and the defects cover basically the surface of ITO. Furthermore, the number of pinholes is small. The analysis of the sample surface and interface further verifies this result by using x-ray photoemission spectroscopy. At the same time, PTCDA is found to have the ability of restraining the diffusion of chemical constituents from ITO to the hole transport layer, which is beneficial to the improvement of the performance and the useful lifetime of the organic light emitting diodes （OLEDs）.
