The acidity of atmospheric aerosols influences fundamental physicochemical processes that affect climate and human health.We recently developed a novel and facilewater-probebased method for directly measuring of the p...The acidity of atmospheric aerosols influences fundamental physicochemical processes that affect climate and human health.We recently developed a novel and facilewater-probebased method for directly measuring of the pH for micrometer-size droplets,providing a promising technique to better understand aerosol acidity in the atmosphere.The complex chemical composition of fine particles in the ambient air,however,poses certain challenges to using a water-probe for pH measurement,including interference from interactions between compositions and the influence of similar compositions on water structure.To explore the universality of our method,it was employed to measure the pH of ammonium,nitrate,carbonate,sulfate,and chloride particles.The pH of particles covering a broad range(0–14)were accurately determined,thereby demonstrating that our method can be generally applied,even to alkaline particles.Furthermore,a standard spectral library was developed by integrating the standard spectra of common hydrated ions extracted through the waterprobe.The library can be employed to identify particle composition and overcome the spectral overlap problem resulting from similar effects.Using the spectral library,all ions were identified and their concentrations were determined,in turn allowing successful pH measurement of multicomponent(ammonium-sulfate-nitrate-chloride)particles.Insights into the synergistic effect of Cl^(–),NO_(3)^(–),and NH_(4)^(+)depletion obtained with our approach revealed the interplay between pH and volatile partitioning.Given the ubiquity of component partitioning and pH variation in particles,the water probemay provide a new perspective on the underlying mechanisms of aerosol aging and aerosol–cloud interaction.展开更多
Si-based multilayer structures are widely used in current microelectronics. During their preparation, some inhomogeneous residual stress is induced, resulting in competition between interface mismatching and surface e...Si-based multilayer structures are widely used in current microelectronics. During their preparation, some inhomogeneous residual stress is induced, resulting in competition between interface mismatching and surface energy and even leading to structure failure. This work presents a methodological study on the measurement of residual stress in a multi-layer semiconductor heterostructure. Scanning electron microscopy（SEM）, micro-Raman spectroscopy（MRS）, and transmission electron microscopy（TEM） were applied to measure the geometric parameters of the multilayer structure. The relationship between the Raman spectrum and the stress/strain on the [100] and [110] crystal orientations was determined to enable surface and crosssection residual stress analyses, respectively. Based on the Raman mapping results, the distribution of residual stress along the depth of the multi-layer heterostructure was successfully obtained.展开更多
We developed a set of in-situ Micro-Raman spectroscopy system for autoclave experimental apparatus because of the scientific significance of in-situ Micro-Raman spectroscopy system under the high-pressure hydrothermal...We developed a set of in-situ Micro-Raman spectroscopy system for autoclave experimental apparatus because of the scientific significance of in-situ Micro-Raman spectroscopy system under the high-pressure hydrothermal condition.We used this system to measure the Raman spectrum of water-fluid and quartz crystal at the temperature ranging from 125 to 420℃.The signal-tonoise ratio of the Raman signal is good.展开更多
BACKGROUND： A variety of methods have been used to identify and distinguish motor and sensory nerves. However, their application is limited clinically due to the complex operation, time consumption, and subjectivity....BACKGROUND： A variety of methods have been used to identify and distinguish motor and sensory nerves. However, their application is limited clinically due to the complex operation, time consumption, and subjectivity. Raman spectroscopy is a minimally invasive method that provides information about molecular structure and constitutions and has been frequently used for tissue identification. OBJECTIVE： To explore a time-efficient method of identifying motor and sensory fascicles in peripheral nerve trunk using laser micro-Raman spectroscopy.DESIGN, TIME AND SETTING： A comparative observation was performed at the Key Laboratory of Excited States Physics in Chinese Academy of Science, Changchun Branch, from October 2004 to October 2005. MATERIALS： JY-HR800 laser confocal micro-Raman spectrometer was purchased from Jobin-Yvon France; 2060-10 argon ion laser was purchased from Spectra-Physics, USA. METHODS： A total of 32 New Zealand rabbits were selected and sacrificed. The roots of spinal nerves were exposed under an operating microscope, and the anterior and posterior roots, approximately 3-5 mm, were dissociated, and frozen as transverse sections of 30 μm thickness. The sections were examined by micro-Raman spectroscopy. MAIN OUTCOME MEASURES： The specific spectral features of motor and sensory fascicles in the Raman spectra. RESULTS： Sections of the same type of nerve fascicle showed reproducibility with similar spectral features. Significant differences in the spectral properties, such as the intensity and breadth of the peak, were found between motor and sensory fascicles in the frequency regions of 1 088, 1 276, 1 439, 1 579, and 1 659 cm^-1. With the peak intensity ratio of 1.06 （/1276//1439） as a standard, we could identify motor fascicles with a sensitivity of 88%, specificity of 94 %, positive predictive value of 93% and negative predictive value of 88%. In the range of 2 700-3 500 cm^-1, the half-peak width of the motor fascicles was narrow and sharp, while that of the sensory fascicles was relatively wider. A total of 91% of the peak features were in accordance with the identification standard. CONCLUSION： Motor and sensory fascicles exhibit different characteristics in Raman spectra, which are constant and reliable. Therefore, it is an effective method to identify nerve fascicles according to the specific spectrum.展开更多
A series of cubic SiC single crystals were heteroepitaxially grown by the hot-wall chemical vapor deposition (CVD) using a HMDS-C3H8-H2 system on 2 inch silicon substrates with the orientations of (100), (111), (110) ...A series of cubic SiC single crystals were heteroepitaxially grown by the hot-wall chemical vapor deposition (CVD) using a HMDS-C3H8-H2 system on 2 inch silicon substrates with the orientations of (100), (111), (110) and (211), respectively. Even though an initial carbonization was carried out to reduce the large lattice mismatch, residual stress could not be completely relieved, partly also due to the difference of their thermal expansion coefficients. Raman scattering studies for the specimens were performed to estimate the internal stress in the SiC epilayer and the substrate. Raman spectra were mapped out on the sample surface as well as on the cross section using an automated x-y stage with a spatial resolution capable of 100 nm. For all the samples, two Raman peaks corresponding to the transverse optical (TO) and longitudinal optical (LO) phonon modes were observed, even though the intensity varied with the polarization configurations. In the SiC epilayers, tensile stresses decrease away from the interface, while compressive stresses exist in the substrate, with the magnitudes dependent on the growth orientation. The lattice strains were discussed in terms of the elastic deformation theory for the comparison.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 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
Optical monitoring of fireballs can provide reconstructions of luminous trajectories and the derivation of heliocentric orbits,whereas spectral observations are able to supply information from an entirely different pe...Optical monitoring of fireballs can provide reconstructions of luminous trajectories and the derivation of heliocentric orbits,whereas spectral observations are able to supply information from an entirely different perspective,with composition and material data.Observing and analyzing a fireball by using both methods enables a complete characterization of its meteorite properties.We simultaneously collected luminous and spectral observations of fireballs through observation networks established in eastern China and the Western Cape of South Africa.The optical observations utilized 180°×180°fisheye cameras,whereas spectral data were recorded by fixing gratings in front of each camera lens on the Allsky7 instrument so that both could monitor fireballs within an all-sky field of view.The spectra had an effective resolution of R=200.During the first year of operation,the network detected spectra from 150 fireballs,most of which recognized at least Mg I and Na I emission lines,and both the spectra and trajectory were recorded for some.Preliminary analysis of four bright fireballs indicated they could be categorized as asteroidal orbits or Halley-type cometary orbits,with spectra classified as normal,Fe-rich,iron,and Na-poor,respectively.One Halley-type fireball belonged to the Perseid meteor shower.For the two fireballs on asteroid-like orbits,orbital comparisons with known near-Earth asteroids were performed using multiple D-criteria(orbital similarity functions).Under the D_(N)criterion,SAFB20250713(iron type)showed a loose possible match with 2021 BD,whereas JsFB20250110(Fe-rich type)exhibited a closer potential similarity with 2017 BK(D_(N)=0.03).Overall,the orbital comparison indicated possible associations but no definitive parent bodies,whereas the spectral characteristics were broadly consistent with the asteroid-like or comet-like nature implied by their orbital classes.展开更多
In this paper,a fast step heterodyne light-induced thermoelastic spectroscopy(SH-LITES)sensor using a high-frequency quartz tuning fork(QTF)with resonant frequency of~100 kHz is reported for the first time.The theoret...In this paper,a fast step heterodyne light-induced thermoelastic spectroscopy(SH-LITES)sensor using a high-frequency quartz tuning fork(QTF)with resonant frequency of~100 kHz is reported for the first time.The theoretical principle of heterodyne LITES(H-LITES)signal generation is analyzed firstly,and an acetylene(C_(2)H_(2))H-LITES sensor is established to verify its performance.Experimental comparisons between the high-frequency QTF and a standard commercial QTF with resonant frequency of~32.768 kHz reveal that the high-frequency QTF exhibits a tenfold faster response time.Specifically,the H-LITES sensor with this QTF achieves a 33 ms measurement cycle,90%shorter than commercial counterparts.Furthermore,The SH-LITES technique is proposed to further shorten the scanning time to 15 ms,which achieves the shortest LITES measurement time known to date.To demonstrate its advantages in dynamic gas detection,an H_(2)O-LITES system integrating both QTF types is constructed for real-time monitoring of H_(2)O concentration during different respiration patterns.Comparative measurements show that the SH-LITES more accurately captures dynamic H_(2)O concentration fluctuations during respiration,outperforming the commercial QTF-based H-LITES sensor in rapid response scenarios.展开更多
The increasing power density of chips poses a significant challenge in the form of material aging for aluminumfilled polydimethylsiloxane(Al/PDMS)composites,which are widely used in thermal interface materials.Despite...The increasing power density of chips poses a significant challenge in the form of material aging for aluminumfilled polydimethylsiloxane(Al/PDMS)composites,which are widely used in thermal interface materials.Despite the growing importance of this issue,the specific mechanisms behind the interfacial aging process remain elusive,hindering a comprehensive grasp of the aging dynamics in these composites.In our research,we have developed an in-situ Raman aging monitoring system that leverages the non-contact and high-resolution capabilities of Raman spectroscopy to study the interface aging process.Our findings indicate a notable decrease in the intensity of the Raman peak as further cross-linking of the molecules during aging,with the most pronounced decline occurring at the interface between aluminum and PDMS.This insight could potentially elucidate why the interface in composite materials is frequently the site of failure during aging.Our study offers a versatile methodology for investigating the interfacial aging of polymer composites,contributing to a broader understanding of the interface behavior in composite materials at the molecular level.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
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
In this work,we develop an extended dissipaton theory that generalizes the environmental couplings beyond the conventional linear and quadratic forms,enabling the treatment of ar-bitrary order of bath couplings.Ap-ply...In this work,we develop an extended dissipaton theory that generalizes the environmental couplings beyond the conventional linear and quadratic forms,enabling the treatment of ar-bitrary order of bath couplings.Ap-plying this theoretical framework to the condensed-phase non-Condon spectroscopy,we demonstrate the in-terplay of anharmonicity,non-Con-don and solvent effects on optical spectra,where the higher-order cou-plings arise from the anharmonicity of nuclear potential surface of the excited state.Precise simulations are carried out with high efficiency on linear absorption spectra involving the above mentioned correlated effects.We exhibit how an anharmonic potential modulates the vibronic feature,offering insights into the role of nonlinear environmental couplings in spectroscopic signatures and exemplifying the success of the extended dissipaton formalism as an exact and efficient method for higher-or-der bath couplings.展开更多
Existing methods for tracing water pollution sources typically integrate three-dimensional excitationemission matrix(3D-EEM)fluorescence spectroscopy with similarity-based matching algorithms.However,these approaches ...Existing methods for tracing water pollution sources typically integrate three-dimensional excitationemission matrix(3D-EEM)fluorescence spectroscopy with similarity-based matching algorithms.However,these approaches exhibit high error rates in borderline cases and necessitate expert manual review,which limits scalability and introduces inconsistencies between algorithmic outputs and expert judgment.To address these limitations,we propose a large vision-language model(VLM)designed as an“expert agent”to automatically refine similarity scores,ensuring alignment with expert decisions and overcoming key application bottlenecks.The model consists of two core components:(1)rule-based similarity calculation module generate initial spectral similarity scores,and(2)pre-trained large vision-language model fine-tuned via supervised learning and reinforcement learning with human feedback(RLHF)to emulate expert assessments.To facilitate training and evaluation,we introduce two expert-annotated datasets,Spec1k and SpecReason,which capture both quantitative corrections and qualitative reasoning patterns,allowing the model to emulate expert decision-making processes.Experimental results demonstrate that our method achieves 81.45%source attribution accuracy,38.24%higher than rule-based and machine learning baselines.Real-world deployment further validates its effectiveness.展开更多
基金supported by the National Natural Science Foundation of China(No.91844000)China Postdoctoral Science Foundation(No.2020M670048).
文摘The acidity of atmospheric aerosols influences fundamental physicochemical processes that affect climate and human health.We recently developed a novel and facilewater-probebased method for directly measuring of the pH for micrometer-size droplets,providing a promising technique to better understand aerosol acidity in the atmosphere.The complex chemical composition of fine particles in the ambient air,however,poses certain challenges to using a water-probe for pH measurement,including interference from interactions between compositions and the influence of similar compositions on water structure.To explore the universality of our method,it was employed to measure the pH of ammonium,nitrate,carbonate,sulfate,and chloride particles.The pH of particles covering a broad range(0–14)were accurately determined,thereby demonstrating that our method can be generally applied,even to alkaline particles.Furthermore,a standard spectral library was developed by integrating the standard spectra of common hydrated ions extracted through the waterprobe.The library can be employed to identify particle composition and overcome the spectral overlap problem resulting from similar effects.Using the spectral library,all ions were identified and their concentrations were determined,in turn allowing successful pH measurement of multicomponent(ammonium-sulfate-nitrate-chloride)particles.Insights into the synergistic effect of Cl^(–),NO_(3)^(–),and NH_(4)^(+)depletion obtained with our approach revealed the interplay between pH and volatile partitioning.Given the ubiquity of component partitioning and pH variation in particles,the water probemay provide a new perspective on the underlying mechanisms of aerosol aging and aerosol–cloud interaction.
基金supported by the National Basic Research Program of China (Grant 2012CB937500)the National Natural Science Foundation of China (Grants 11422219, 11227202, 11372217, 11272232)+1 种基金the Program for New Century Excellent Talents in University (Grant NCET-13)China Scholarship Council (201308120092)
文摘Si-based multilayer structures are widely used in current microelectronics. During their preparation, some inhomogeneous residual stress is induced, resulting in competition between interface mismatching and surface energy and even leading to structure failure. This work presents a methodological study on the measurement of residual stress in a multi-layer semiconductor heterostructure. Scanning electron microscopy（SEM）, micro-Raman spectroscopy（MRS）, and transmission electron microscopy（TEM） were applied to measure the geometric parameters of the multilayer structure. The relationship between the Raman spectrum and the stress/strain on the [100] and [110] crystal orientations was determined to enable surface and crosssection residual stress analyses, respectively. Based on the Raman mapping results, the distribution of residual stress along the depth of the multi-layer heterostructure was successfully obtained.
基金supported by the National Key R&D Program of China(Grant No.2016YFC0600104)the Strategic Priority Research Program(B)of the Chinese Academy of Sciences(XDB 18010401)。
文摘We developed a set of in-situ Micro-Raman spectroscopy system for autoclave experimental apparatus because of the scientific significance of in-situ Micro-Raman spectroscopy system under the high-pressure hydrothermal condition.We used this system to measure the Raman spectrum of water-fluid and quartz crystal at the temperature ranging from 125 to 420℃.The signal-tonoise ratio of the Raman signal is good.
文摘BACKGROUND： A variety of methods have been used to identify and distinguish motor and sensory nerves. However, their application is limited clinically due to the complex operation, time consumption, and subjectivity. Raman spectroscopy is a minimally invasive method that provides information about molecular structure and constitutions and has been frequently used for tissue identification. OBJECTIVE： To explore a time-efficient method of identifying motor and sensory fascicles in peripheral nerve trunk using laser micro-Raman spectroscopy.DESIGN, TIME AND SETTING： A comparative observation was performed at the Key Laboratory of Excited States Physics in Chinese Academy of Science, Changchun Branch, from October 2004 to October 2005. MATERIALS： JY-HR800 laser confocal micro-Raman spectrometer was purchased from Jobin-Yvon France; 2060-10 argon ion laser was purchased from Spectra-Physics, USA. METHODS： A total of 32 New Zealand rabbits were selected and sacrificed. The roots of spinal nerves were exposed under an operating microscope, and the anterior and posterior roots, approximately 3-5 mm, were dissociated, and frozen as transverse sections of 30 μm thickness. The sections were examined by micro-Raman spectroscopy. MAIN OUTCOME MEASURES： The specific spectral features of motor and sensory fascicles in the Raman spectra. RESULTS： Sections of the same type of nerve fascicle showed reproducibility with similar spectral features. Significant differences in the spectral properties, such as the intensity and breadth of the peak, were found between motor and sensory fascicles in the frequency regions of 1 088, 1 276, 1 439, 1 579, and 1 659 cm^-1. With the peak intensity ratio of 1.06 （/1276//1439） as a standard, we could identify motor fascicles with a sensitivity of 88%, specificity of 94 %, positive predictive value of 93% and negative predictive value of 88%. In the range of 2 700-3 500 cm^-1, the half-peak width of the motor fascicles was narrow and sharp, while that of the sensory fascicles was relatively wider. A total of 91% of the peak features were in accordance with the identification standard. CONCLUSION： Motor and sensory fascicles exhibit different characteristics in Raman spectra, which are constant and reliable. Therefore, it is an effective method to identify nerve fascicles according to the specific spectrum.
文摘A series of cubic SiC single crystals were heteroepitaxially grown by the hot-wall chemical vapor deposition (CVD) using a HMDS-C3H8-H2 system on 2 inch silicon substrates with the orientations of (100), (111), (110) and (211), respectively. Even though an initial carbonization was carried out to reduce the large lattice mismatch, residual stress could not be completely relieved, partly also due to the difference of their thermal expansion coefficients. Raman scattering studies for the specimens were performed to estimate the internal stress in the SiC epilayer and the substrate. Raman spectra were mapped out on the sample surface as well as on the cross section using an automated x-y stage with a spatial resolution capable of 100 nm. For all the samples, two Raman peaks corresponding to the transverse optical (TO) and longitudinal optical (LO) phonon modes were observed, even though the intensity varied with the polarization configurations. In the SiC epilayers, tensile stresses decrease away from the interface, while compressive stresses exist in the substrate, with the magnitudes dependent on the growth orientation. The lattice strains were discussed in terms of the elastic deformation theory for the comparison.
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.
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supported by the Science and Technology Project of Qinghai Province(Grant No.2025-ZJ-T0)the National Key Research and Development Program of China(Grant No.2023YFE0109900)the Minor Planet Foundation of China.
文摘Optical monitoring of fireballs can provide reconstructions of luminous trajectories and the derivation of heliocentric orbits,whereas spectral observations are able to supply information from an entirely different perspective,with composition and material data.Observing and analyzing a fireball by using both methods enables a complete characterization of its meteorite properties.We simultaneously collected luminous and spectral observations of fireballs through observation networks established in eastern China and the Western Cape of South Africa.The optical observations utilized 180°×180°fisheye cameras,whereas spectral data were recorded by fixing gratings in front of each camera lens on the Allsky7 instrument so that both could monitor fireballs within an all-sky field of view.The spectra had an effective resolution of R=200.During the first year of operation,the network detected spectra from 150 fireballs,most of which recognized at least Mg I and Na I emission lines,and both the spectra and trajectory were recorded for some.Preliminary analysis of four bright fireballs indicated they could be categorized as asteroidal orbits or Halley-type cometary orbits,with spectra classified as normal,Fe-rich,iron,and Na-poor,respectively.One Halley-type fireball belonged to the Perseid meteor shower.For the two fireballs on asteroid-like orbits,orbital comparisons with known near-Earth asteroids were performed using multiple D-criteria(orbital similarity functions).Under the D_(N)criterion,SAFB20250713(iron type)showed a loose possible match with 2021 BD,whereas JsFB20250110(Fe-rich type)exhibited a closer potential similarity with 2017 BK(D_(N)=0.03).Overall,the orbital comparison indicated possible associations but no definitive parent bodies,whereas the spectral characteristics were broadly consistent with the asteroid-like or comet-like nature implied by their orbital classes.
基金financial supports from the National Natural Science Foundation of China(Grant No.62335006,62275065,624B2050,62022032,and 62405078)Open Subject of Hebei Key Laboratory of Advanced Laser Technology and Equipment(HBKL-ALTE2025001)+2 种基金Heilongjiang Postdoctoral Fund(Grant No.LBH-Z23144 and LBH-Z24155)Natural Science Foundation of Heilongjiang Province(Grant No.LH2024F031)China Postdoctoral Science Foundation(Grant No.2024M764172).
文摘In this paper,a fast step heterodyne light-induced thermoelastic spectroscopy(SH-LITES)sensor using a high-frequency quartz tuning fork(QTF)with resonant frequency of~100 kHz is reported for the first time.The theoretical principle of heterodyne LITES(H-LITES)signal generation is analyzed firstly,and an acetylene(C_(2)H_(2))H-LITES sensor is established to verify its performance.Experimental comparisons between the high-frequency QTF and a standard commercial QTF with resonant frequency of~32.768 kHz reveal that the high-frequency QTF exhibits a tenfold faster response time.Specifically,the H-LITES sensor with this QTF achieves a 33 ms measurement cycle,90%shorter than commercial counterparts.Furthermore,The SH-LITES technique is proposed to further shorten the scanning time to 15 ms,which achieves the shortest LITES measurement time known to date.To demonstrate its advantages in dynamic gas detection,an H_(2)O-LITES system integrating both QTF types is constructed for real-time monitoring of H_(2)O concentration during different respiration patterns.Comparative measurements show that the SH-LITES more accurately captures dynamic H_(2)O concentration fluctuations during respiration,outperforming the commercial QTF-based H-LITES sensor in rapid response scenarios.
基金supported by the National Natural Science Foundation of China(No.52303092)Talent Recruitment Project of Guangdong Province(No.2023QN10X078)+2 种基金Open Project of Yunnan Precious Metals Laboratory Co.,Ltd(No.YPML-2023050278)National Key R&D Project from Ministry of Science and Technology of China(No.2022YFA1203100)Shenzhen Science and Technology Research Funding(No.JCYJ20200109114401708)。
文摘The increasing power density of chips poses a significant challenge in the form of material aging for aluminumfilled polydimethylsiloxane(Al/PDMS)composites,which are widely used in thermal interface materials.Despite the growing importance of this issue,the specific mechanisms behind the interfacial aging process remain elusive,hindering a comprehensive grasp of the aging dynamics in these composites.In our research,we have developed an in-situ Raman aging monitoring system that leverages the non-contact and high-resolution capabilities of Raman spectroscopy to study the interface aging process.Our findings indicate a notable decrease in the intensity of the Raman peak as further cross-linking of the molecules during aging,with the most pronounced decline occurring at the interface between aluminum and PDMS.This insight could potentially elucidate why the interface in composite materials is frequently the site of failure during aging.Our study offers a versatile methodology for investigating the interfacial aging of polymer composites,contributing to a broader understanding of the interface behavior in composite materials at the molecular level.
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.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supported by the National Natural Sci-ence Foundation of China(Nos.22373091,224B2305,and 22573099).
文摘In this work,we develop an extended dissipaton theory that generalizes the environmental couplings beyond the conventional linear and quadratic forms,enabling the treatment of ar-bitrary order of bath couplings.Ap-plying this theoretical framework to the condensed-phase non-Condon spectroscopy,we demonstrate the in-terplay of anharmonicity,non-Con-don and solvent effects on optical spectra,where the higher-order cou-plings arise from the anharmonicity of nuclear potential surface of the excited state.Precise simulations are carried out with high efficiency on linear absorption spectra involving the above mentioned correlated effects.We exhibit how an anharmonic potential modulates the vibronic feature,offering insights into the role of nonlinear environmental couplings in spectroscopic signatures and exemplifying the success of the extended dissipaton formalism as an exact and efficient method for higher-or-der bath couplings.
文摘Existing methods for tracing water pollution sources typically integrate three-dimensional excitationemission matrix(3D-EEM)fluorescence spectroscopy with similarity-based matching algorithms.However,these approaches exhibit high error rates in borderline cases and necessitate expert manual review,which limits scalability and introduces inconsistencies between algorithmic outputs and expert judgment.To address these limitations,we propose a large vision-language model(VLM)designed as an“expert agent”to automatically refine similarity scores,ensuring alignment with expert decisions and overcoming key application bottlenecks.The model consists of two core components:(1)rule-based similarity calculation module generate initial spectral similarity scores,and(2)pre-trained large vision-language model fine-tuned via supervised learning and reinforcement learning with human feedback(RLHF)to emulate expert assessments.To facilitate training and evaluation,we introduce two expert-annotated datasets,Spec1k and SpecReason,which capture both quantitative corrections and qualitative reasoning patterns,allowing the model to emulate expert decision-making processes.Experimental results demonstrate that our method achieves 81.45%source attribution accuracy,38.24%higher than rule-based and machine learning baselines.Real-world deployment further validates its effectiveness.
