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
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 presence of a positive deep surgical margin in tongue squamous cell carcinoma(TSCC)significantly elevates the risk of local recurrence.Therefore,a prompt and precise intraoperative assessment of margin status is i...The presence of a positive deep surgical margin in tongue squamous cell carcinoma(TSCC)significantly elevates the risk of local recurrence.Therefore,a prompt and precise intraoperative assessment of margin status is imperative to ensure thorough tumor resection.In this study,we integrate Raman imaging technology with an artificial intelligence(AI)generative model,proposing an innovative approach for intraoperative margin status diagnosis.This method utilizes Raman imaging to swiftly and non-invasively capture tissue Raman images,which are then transformed into hematoxylin-eosin(H&E)-stained histopathological images using an AI generative model for histopathological diagnosis.The generated H&E-stained images clearly illustrate the tissue’s pathological conditions.Independently reviewed by three pathologists,the overall diagnostic accuracy for distinguishing between tumor tissue and normal muscle tissue reaches 86.7%.Notably,it outperforms current clinical practices,especially in TSCC with positive lymph node metastasis or moderately differentiated grades.This advancement highlights the potential of AI-enhanced Raman imaging to significantly improve intraoperative assessments and surgical margin evaluations,promising a versatile diagnostic tool beyond TSCC.展开更多
Edge structures are ubiquitous in the processing and fabrication of various optoelectronic devices.Novel physical properties and enhanced light–matter interactions are anticipated to occur at crystal edges due to the...Edge structures are ubiquitous in the processing and fabrication of various optoelectronic devices.Novel physical properties and enhanced light–matter interactions are anticipated to occur at crystal edges due to the broken spatial translational symmetry.However,the intensity of first-order Raman scattering at crystal edges has been rarely explored,although the mechanical stress and edge characteristics have been thoroughly studied by the Raman peak shift and the spectral features of the edge-related Raman modes.Here,by taking Ga As crystal with a well-defined edge as an example,we reveal the intensity enhancement of Raman-active modes and the emergence of Raman-forbidden modes under specific polarization configurations at the edge.This is attributed to the presence of a hot spot at the edge due to the redistributed electromagnetic fields and electromagnetic wave propagations of incident laser and Raman signal near the edge,which are confirmed by the finite-difference time-domain simulations.Spatially-resolved Raman intensities of both Raman-active and Raman-forbidden modes near the edge are calculated based on the redistributed electromagnetic fields,which quantitatively reproduce the corresponding experimental results.These findings offer new insights into the intensity enhancement of Raman scattering at crystal edges and present a new avenue to manipulate light–matter interactions of crystal by manufacturing various types of edges and to characterize the edge structures in photonic and optoelectronic devices.展开更多
Lipids play an important role in the regulation of cell life processes.Although there are various lipid detection methods,Raman spectroscopy,a non-invasive technique,provides the detailed chemical composition of lipid...Lipids play an important role in the regulation of cell life processes.Although there are various lipid detection methods,Raman spectroscopy,a non-invasive technique,provides the detailed chemical composition of lipid profiles without a complex sample preparation procedure and possesses greater potential in basic biology,clinical diagnosis and disease therapy.In this review,we summarized the characteristics and advantages of Raman-based techniques and their primary contribution to illustrating cellular lipid metabolism.展开更多
Stimulated Raman scattering(SRS)under a new ignition path that combines the advantages of direct-drive(DD)and indirect-drive(ID)schemes is investigated experimentally at the Shenguang-100 kJ facility.The results show ...Stimulated Raman scattering(SRS)under a new ignition path that combines the advantages of direct-drive(DD)and indirect-drive(ID)schemes is investigated experimentally at the Shenguang-100 kJ facility.The results show that collective SRS in the plasma produced by ablating a polyimide film is detected for the ID beams,but is suppressed by adding a toe before the main pulse of the ID beams.The toe also strongly influences SRS of both the ID and DD beams excited in the plasma generated in the hohlraum.When a toe is used,the SRS spectra of the DD beams show that SRS tends to be excited in lower plasma density,which will result in a lower risk of super-hot electrons.Measurements of hot electrons support this conclusion.This research will help us produce a better pulse design for this new ignition path.展开更多
The layered van der Waals(vdW)ferroelectric CuInP_(2)S_(6) (CIPS)exhibits unique cation-hopping-driven phenomena that bring about unconventional properties with intriguing mechanisms and hold promise for advanced appl...The layered van der Waals(vdW)ferroelectric CuInP_(2)S_(6) (CIPS)exhibits unique cation-hopping-driven phenomena that bring about unconventional properties with intriguing mechanisms and hold promise for advanced applications in nanoelectronics.However,an explicit analysis of its lattice dynamics and vibrational symmetries,pivotal for understanding the material’s peculiar ferroelectric and ferroionic behaviors,remains incomplete.Here,we employ angle-resolved polarized Raman spectroscopy in concert with first-principles calculations to systematically unravel the anisotropic lattice vibrations of CIPS single crystals.By analyzing the polarization-dependent Raman intensities,we determine the symmetry assignments and Raman tensors of all major vibrational modes,revealing good agreement with theoretical predictions.Furthermore,we demonstrate the utility of Raman spectroscopy as a sensitive and non-invasive probe for structural and ferroelectric order evolution by examining temperature-driven phase transitions and thickness-dependent polarization suppression in CIPS.Our findings establish a foundational framework for correlating lattice dynamics with functional properties in CIPS and provide a methodological blueprint for studying other vdW ferroelectrics.展开更多
Recent experiments at the National Ignition Facility and theoretical modeling suggest that side stimulated Raman scattering(SSRS)instability could reduce laser–plasma coupling and generate considerable fluxes of supr...Recent experiments at the National Ignition Facility and theoretical modeling suggest that side stimulated Raman scattering(SSRS)instability could reduce laser–plasma coupling and generate considerable fluxes of suprathermal hot electrons under interaction conditions envisaged for direct-drive schemes for inertial confinement fusion.Nonetheless,SSRS remains to date one of the least understood parametric instabilities.Here,we report the first angularly and spectrally resolved measurements of scattered light at laser intensities relevant for the shock ignition scheme(I×10^(16)W/cm^(2)),showing significant SSRS growth in the direction perpendicular to the laser polarization.Modification of the focal spot shape and orientation,obtained by using two different random phase plates,and of the density gradient of the plasma,by utilizing exploding foil targets of different thicknesses,clearly reveals a different dependence of backward SRS(BSRS)and SSRS on experimental parameters.While convective BSRS scales with plasma density scale length,as expected by linear theory,the growth of SSRS depends on the spot extension in the direction perpendicular to laser polarization.Our analysis therefore demonstrates that under current experimental conditions,with density scale lengths L_(n)≈60–120μm and spot sizes FWHM≈40–100μm,SSRS is limited by laser beam size rather than by the density scale length of the plasma.展开更多
Glucose molecules are of great significance being one of the most important molecules in metabolic chain.However,due to the small Raman scattering cross-section and weak/non-adsorption on bare metals,accurately obtain...Glucose molecules are of great significance being one of the most important molecules in metabolic chain.However,due to the small Raman scattering cross-section and weak/non-adsorption on bare metals,accurately obtaining their"fingerprint information"remains a huge obstacle.Herein,we developed a tip-enhanced Raman scattering(TERS)technique to address this challenge.Adopting an optical fiber radial vector mode internally illuminates the plasmonic fiber tip to effectively suppress the background noise while generating a strong electric-field enhanced tip hotspot.Furthermore,the tip hotspot approaching the glucose molecules was manipulated via the shear-force feedback to provide more freedom for selecting substrates.Consequently,our TERS technique achieves the visualization of all Raman modes of glucose molecules within spectral window of 400-3200 cm^(-1),which is not achievable through the far-field/surface-enhanced Raman,or the existing TERS techniques.Our TERS technique offers a powerful tool for accurately identifying Raman scattering of molecules,paving the way for biomolecular analysis.展开更多
In this study,we developed a single-beam optical trap-based surface-enhanced Raman scattering(SERS)optofluidic molecular fingerprint spectroscopy detection system.This system utilizes a single-beam optical trap to con...In this study,we developed a single-beam optical trap-based surface-enhanced Raman scattering(SERS)optofluidic molecular fingerprint spectroscopy detection system.This system utilizes a single-beam optical trap to concentrate free silver nanoparticles(AgNPs)within an optofluidic chip,significantly enhancing SERS performance.We investigated the optical field distribution characteristics within the tapered fiber using COMSOL simulation software and established a MATLAB simulation model to validate the single-beam optical trap's effectiveness in capturing AgNPs,demonstrating the theoretical feasibility of our approach.To verify the particle capture efficacy of the system,we experimentally controlled the optical trap's on-off state to manage the capture and release of particles precisely.The experimental results indicated that the Raman signal intensity in the capture state was significantly higher than in the non-capture state,confirming that the single-beam optical trap effectively enhances the SERS detection capability of the optofluidic detection system.Furthermore,we employed Raman mapping techniques to investigate the impact of the capture area on the SERS effect,revealing that the spectral intensity of molecular fingerprints in the laser-trapping region is significantly improved.We successfully detected the Raman spectrum of crystal violet at a concentration of 10^(−9)mol/L and pesticide thiram at a concentration of 10^(−5)mol/L,further demonstrating the ability of the single-beam optical trap in enhancing the molecular fingerprint spectrum identification capability of the SERS optofluidic chips.The optical trapping SERS optofluidic detection system developed in this study,as a key component of an integrated optoelectronic sensing system,holds the potential for integration with portable high-power lasers and high-performance Raman spectrometers.This integration is expected to advance highly integrated technologies and significantly enhance the overall performance and portability of optoelectronic sensing systems.展开更多
BACKGROUND Esophageal squamous cell carcinoma is a major histological subtype of esophageal cancer.Many molecular genetic changes are associated with its occurrence.Raman spectroscopy has become a new method for the e...BACKGROUND Esophageal squamous cell carcinoma is a major histological subtype of esophageal cancer.Many molecular genetic changes are associated with its occurrence.Raman spectroscopy has become a new method for the early diagnosis of tumors because it can reflect the structures of substances and their changes at the molecular level.AIM To detect alterations in Raman spectral information across different stages of esophageal neoplasia.METHODS Different grades of esophageal lesions were collected,and a total of 360 groups of Raman spectrum data were collected.A 1D-transformer network model was proposed to handle the task of classifying the spectral data of esophageal squamous cell carcinoma.In addition,a deep learning model was applied to visualize the Raman spectral data and interpret their molecular characteristics.RESULTS A comparison among Raman spectral data with different pathological grades and a visual analysis revealed that the Raman peaks with significant differences were concentrated mainly at 1095 cm^(-1)(DNA,symmetric PO,and stretching vibration),1132 cm^(-1)(cytochrome c),1171 cm^(-1)(acetoacetate),1216 cm^(-1)(amide III),and 1315 cm^(-1)(glycerol).A comparison among the training results of different models revealed that the 1Dtransformer network performed best.A 93.30%accuracy value,a 96.65%specificity value,a 93.30%sensitivity value,and a 93.17%F1 score were achieved.CONCLUSION Raman spectroscopy revealed significantly different waveforms for the different stages of esophageal neoplasia.The combination of Raman spectroscopy and deep learning methods could significantly improve the accuracy of classification.展开更多
Raman spectroscopy offers a great power to detect,analyze and identify molecules,and monitor their temporal dynamics and evolution when combined with single-molecule surface-enhanced Raman scattering(SM-SERS)substrate...Raman spectroscopy offers a great power to detect,analyze and identify molecules,and monitor their temporal dynamics and evolution when combined with single-molecule surface-enhanced Raman scattering(SM-SERS)substrates.Here we present a SM-SERS scheme that involves simultaneously giant chemical enhancement from WS22D materials,giant electromagnetic enhancement from plasmonic nanogap hot spot,and inhibition of molecular fluorescence influence under near-infrared laser illumination.Remarkably we find Coulomb attraction between analyte and gold nanoparticle can trigger spontaneous formation of molecule-hotspot pairing with high precision,stability and robustness.The scheme has enabled realization of universal,robust,fast,and large-scale uniform SM-SERS detection for three Raman molecules of rhodamine B,rhodamine 6G,and crystal violet with a very low detection limit of 10−16 M and at a very fast spectrum acquisition time of 50 ms.展开更多
Quantitative detection of trace small-sized nanoplastics(<100 nm)remains a significant challenge in surface-enhanced Raman scattering(SERS).To tackle this issue,we developed a hydrophobic CuO@Ag nanowire substrate ...Quantitative detection of trace small-sized nanoplastics(<100 nm)remains a significant challenge in surface-enhanced Raman scattering(SERS).To tackle this issue,we developed a hydrophobic CuO@Ag nanowire substrate and introduced a multiplex-feature analysis strategy based on the coffee ring effect.This substrate not only offers high Raman enhancement but also exhibits a high probability of detection(POD),enabling rapid and accurate identification of 50 nm polystyrene nanoplastics over a broad concentration range(1–10−10 wt%).Importantly,experimental results reveal a strong correlation between the coffee ring formation and the concentration of nanoplastic dispersion.By incorporating Raman signal intensity,coffee ring diameter,and POD as combined features,we established a machine learning-based mapping between nanoplastic concentration and coffee ring characteristics,allowing precise predictions of dispersion concentration.The mean squared error of these predictions is remarkably low,ranging from 0.21 to 0.54,representing a 19 fold improvement in accuracy compared to traditional linear regression-based methods.This strategy effectively integrates SERS with wettability modification techniques,ensuring high sensitivity and fingerprinting capabilities,while addressing the limitations of Raman signal intensity in accurately reflecting concentration changes at ultra-low levels,providing a new idea for precise SERS measurements of nanoplastics.展开更多
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 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 Science Foundation of China(Grant Nos.82272955 and 22203057)the Natural Science Foundation of Fujian Province(Grant No.2021J011361).
文摘The presence of a positive deep surgical margin in tongue squamous cell carcinoma(TSCC)significantly elevates the risk of local recurrence.Therefore,a prompt and precise intraoperative assessment of margin status is imperative to ensure thorough tumor resection.In this study,we integrate Raman imaging technology with an artificial intelligence(AI)generative model,proposing an innovative approach for intraoperative margin status diagnosis.This method utilizes Raman imaging to swiftly and non-invasively capture tissue Raman images,which are then transformed into hematoxylin-eosin(H&E)-stained histopathological images using an AI generative model for histopathological diagnosis.The generated H&E-stained images clearly illustrate the tissue’s pathological conditions.Independently reviewed by three pathologists,the overall diagnostic accuracy for distinguishing between tumor tissue and normal muscle tissue reaches 86.7%.Notably,it outperforms current clinical practices,especially in TSCC with positive lymph node metastasis or moderately differentiated grades.This advancement highlights the potential of AI-enhanced Raman imaging to significantly improve intraoperative assessments and surgical margin evaluations,promising a versatile diagnostic tool beyond TSCC.
基金Project supported by the National Key Research and Development Program of China(Grant No.2023YFA1407000)the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB0460000)+4 种基金the National Natural Science Foundation of China(Grant Nos.12322401,12127807,and 12393832)CAS Key Research Program of Frontier Sciences(Grant No.ZDBS-LY-SLH004)Beijing Nova Program(Grant No.20230484301)Youth Innovation Promotion Association,Chinese Academy of Sciences(Grant No.2023125)CAS Project for Young Scientists in Basic Research(Grant No.YSBR-026)。
文摘Edge structures are ubiquitous in the processing and fabrication of various optoelectronic devices.Novel physical properties and enhanced light–matter interactions are anticipated to occur at crystal edges due to the broken spatial translational symmetry.However,the intensity of first-order Raman scattering at crystal edges has been rarely explored,although the mechanical stress and edge characteristics have been thoroughly studied by the Raman peak shift and the spectral features of the edge-related Raman modes.Here,by taking Ga As crystal with a well-defined edge as an example,we reveal the intensity enhancement of Raman-active modes and the emergence of Raman-forbidden modes under specific polarization configurations at the edge.This is attributed to the presence of a hot spot at the edge due to the redistributed electromagnetic fields and electromagnetic wave propagations of incident laser and Raman signal near the edge,which are confirmed by the finite-difference time-domain simulations.Spatially-resolved Raman intensities of both Raman-active and Raman-forbidden modes near the edge are calculated based on the redistributed electromagnetic fields,which quantitatively reproduce the corresponding experimental results.These findings offer new insights into the intensity enhancement of Raman scattering at crystal edges and present a new avenue to manipulate light–matter interactions of crystal by manufacturing various types of edges and to characterize the edge structures in photonic and optoelectronic devices.
基金supported by the National Natural Science Foundation of China(Grant NOs.:82374169,and 82074085).
文摘Lipids play an important role in the regulation of cell life processes.Although there are various lipid detection methods,Raman spectroscopy,a non-invasive technique,provides the detailed chemical composition of lipid profiles without a complex sample preparation procedure and possesses greater potential in basic biology,clinical diagnosis and disease therapy.In this review,we summarized the characteristics and advantages of Raman-based techniques and their primary contribution to illustrating cellular lipid metabolism.
基金supported by the National Natural Science Foundation of China(Grant Nos.12205274,12275251,12105270,12205272,12305262,and 12035002)the National Key Laboratory of Plasma Physics(Grant No.JCKYS2024212803)+2 种基金the Fund of the National Key Laboratory of Plasma Physics(Grant No.6142A04230103)the National Key R&D Program of China(Grant No.2023YFA1608400)the National Security Academic Fund(Grant No.U2430207).
文摘Stimulated Raman scattering(SRS)under a new ignition path that combines the advantages of direct-drive(DD)and indirect-drive(ID)schemes is investigated experimentally at the Shenguang-100 kJ facility.The results show that collective SRS in the plasma produced by ablating a polyimide film is detected for the ID beams,but is suppressed by adding a toe before the main pulse of the ID beams.The toe also strongly influences SRS of both the ID and DD beams excited in the plasma generated in the hohlraum.When a toe is used,the SRS spectra of the DD beams show that SRS tends to be excited in lower plasma density,which will result in a lower risk of super-hot electrons.Measurements of hot electrons support this conclusion.This research will help us produce a better pulse design for this new ignition path.
基金supported by the National Natural Science Foundation of China(Grant Nos.12474089,12574102 for L.Y.and L.F.,and 12404102 for J.Z.)the Priority Academic Program Development(PAPD)of Jiangsu Higher Education Institutions(for L.Y.and L.F.)+2 种基金the Natural Science Foundation of the Jiangsu Province(Grant No.BK20230806 for J.Z.)Southeast University Interdisciplinary Research Program for Young Scholars(Grant No.2024FGC1008 for J.Z.)the support by the State Key Laboratory of Solid State Microstructures(Nanjing University)(No.M37067)。
文摘The layered van der Waals(vdW)ferroelectric CuInP_(2)S_(6) (CIPS)exhibits unique cation-hopping-driven phenomena that bring about unconventional properties with intriguing mechanisms and hold promise for advanced applications in nanoelectronics.However,an explicit analysis of its lattice dynamics and vibrational symmetries,pivotal for understanding the material’s peculiar ferroelectric and ferroionic behaviors,remains incomplete.Here,we employ angle-resolved polarized Raman spectroscopy in concert with first-principles calculations to systematically unravel the anisotropic lattice vibrations of CIPS single crystals.By analyzing the polarization-dependent Raman intensities,we determine the symmetry assignments and Raman tensors of all major vibrational modes,revealing good agreement with theoretical predictions.Furthermore,we demonstrate the utility of Raman spectroscopy as a sensitive and non-invasive probe for structural and ferroelectric order evolution by examining temperature-driven phase transitions and thickness-dependent polarization suppression in CIPS.Our findings establish a foundational framework for correlating lattice dynamics with functional properties in CIPS and provide a methodological blueprint for studying other vdW ferroelectrics.
基金financial support from the LASERLAB-EUROPE Access to Research Infrastructure Activity (Application No. 23068)carried out within the framework of EUROfusion Enabling Research Projects AWP21-ENR-01-CEA02 and AWP24-ENR-IFE-02-CEA-02+3 种基金received funding from Euratom Research and Training Programme 2021–2025 under Grant No. 633053supported by the Ministry of Youth and Sports of the Czech Republic [Project No. LM2023068 (PALS RI)]by the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant Nos. XDA25030200 and XDA25010100)supported by COST (European Cooperation in Science and Technology) through Action CA21128 PROBONO (PROton BOron Nuclear Fusion: from energy production to medical applicatiOns)
文摘Recent experiments at the National Ignition Facility and theoretical modeling suggest that side stimulated Raman scattering(SSRS)instability could reduce laser–plasma coupling and generate considerable fluxes of suprathermal hot electrons under interaction conditions envisaged for direct-drive schemes for inertial confinement fusion.Nonetheless,SSRS remains to date one of the least understood parametric instabilities.Here,we report the first angularly and spectrally resolved measurements of scattered light at laser intensities relevant for the shock ignition scheme(I×10^(16)W/cm^(2)),showing significant SSRS growth in the direction perpendicular to the laser polarization.Modification of the focal spot shape and orientation,obtained by using two different random phase plates,and of the density gradient of the plasma,by utilizing exploding foil targets of different thicknesses,clearly reveals a different dependence of backward SRS(BSRS)and SSRS on experimental parameters.While convective BSRS scales with plasma density scale length,as expected by linear theory,the growth of SSRS depends on the spot extension in the direction perpendicular to laser polarization.Our analysis therefore demonstrates that under current experimental conditions,with density scale lengths L_(n)≈60–120μm and spot sizes FWHM≈40–100μm,SSRS is limited by laser beam size rather than by the density scale length of the plasma.
基金supported by National Natural Science Foundation of China(12374358,91950207)Guangdong Basic and Applied Basic Research Foundation(2024A1515010420).
文摘Glucose molecules are of great significance being one of the most important molecules in metabolic chain.However,due to the small Raman scattering cross-section and weak/non-adsorption on bare metals,accurately obtaining their"fingerprint information"remains a huge obstacle.Herein,we developed a tip-enhanced Raman scattering(TERS)technique to address this challenge.Adopting an optical fiber radial vector mode internally illuminates the plasmonic fiber tip to effectively suppress the background noise while generating a strong electric-field enhanced tip hotspot.Furthermore,the tip hotspot approaching the glucose molecules was manipulated via the shear-force feedback to provide more freedom for selecting substrates.Consequently,our TERS technique achieves the visualization of all Raman modes of glucose molecules within spectral window of 400-3200 cm^(-1),which is not achievable through the far-field/surface-enhanced Raman,or the existing TERS techniques.Our TERS technique offers a powerful tool for accurately identifying Raman scattering of molecules,paving the way for biomolecular analysis.
基金financial supports from National Natural Science Foundation of China(62175023).
文摘In this study,we developed a single-beam optical trap-based surface-enhanced Raman scattering(SERS)optofluidic molecular fingerprint spectroscopy detection system.This system utilizes a single-beam optical trap to concentrate free silver nanoparticles(AgNPs)within an optofluidic chip,significantly enhancing SERS performance.We investigated the optical field distribution characteristics within the tapered fiber using COMSOL simulation software and established a MATLAB simulation model to validate the single-beam optical trap's effectiveness in capturing AgNPs,demonstrating the theoretical feasibility of our approach.To verify the particle capture efficacy of the system,we experimentally controlled the optical trap's on-off state to manage the capture and release of particles precisely.The experimental results indicated that the Raman signal intensity in the capture state was significantly higher than in the non-capture state,confirming that the single-beam optical trap effectively enhances the SERS detection capability of the optofluidic detection system.Furthermore,we employed Raman mapping techniques to investigate the impact of the capture area on the SERS effect,revealing that the spectral intensity of molecular fingerprints in the laser-trapping region is significantly improved.We successfully detected the Raman spectrum of crystal violet at a concentration of 10^(−9)mol/L and pesticide thiram at a concentration of 10^(−5)mol/L,further demonstrating the ability of the single-beam optical trap in enhancing the molecular fingerprint spectrum identification capability of the SERS optofluidic chips.The optical trapping SERS optofluidic detection system developed in this study,as a key component of an integrated optoelectronic sensing system,holds the potential for integration with portable high-power lasers and high-performance Raman spectrometers.This integration is expected to advance highly integrated technologies and significantly enhance the overall performance and portability of optoelectronic sensing systems.
基金Supported by Beijing Hospitals Authority Youth Programme,No.QML20200505.
文摘BACKGROUND Esophageal squamous cell carcinoma is a major histological subtype of esophageal cancer.Many molecular genetic changes are associated with its occurrence.Raman spectroscopy has become a new method for the early diagnosis of tumors because it can reflect the structures of substances and their changes at the molecular level.AIM To detect alterations in Raman spectral information across different stages of esophageal neoplasia.METHODS Different grades of esophageal lesions were collected,and a total of 360 groups of Raman spectrum data were collected.A 1D-transformer network model was proposed to handle the task of classifying the spectral data of esophageal squamous cell carcinoma.In addition,a deep learning model was applied to visualize the Raman spectral data and interpret their molecular characteristics.RESULTS A comparison among Raman spectral data with different pathological grades and a visual analysis revealed that the Raman peaks with significant differences were concentrated mainly at 1095 cm^(-1)(DNA,symmetric PO,and stretching vibration),1132 cm^(-1)(cytochrome c),1171 cm^(-1)(acetoacetate),1216 cm^(-1)(amide III),and 1315 cm^(-1)(glycerol).A comparison among the training results of different models revealed that the 1Dtransformer network performed best.A 93.30%accuracy value,a 96.65%specificity value,a 93.30%sensitivity value,and a 93.17%F1 score were achieved.CONCLUSION Raman spectroscopy revealed significantly different waveforms for the different stages of esophageal neoplasia.The combination of Raman spectroscopy and deep learning methods could significantly improve the accuracy of classification.
基金financial support from Science and Technology Project of Guangdong(2020B010190001)National Natural Science Foundation(12434016).
文摘Raman spectroscopy offers a great power to detect,analyze and identify molecules,and monitor their temporal dynamics and evolution when combined with single-molecule surface-enhanced Raman scattering(SM-SERS)substrates.Here we present a SM-SERS scheme that involves simultaneously giant chemical enhancement from WS22D materials,giant electromagnetic enhancement from plasmonic nanogap hot spot,and inhibition of molecular fluorescence influence under near-infrared laser illumination.Remarkably we find Coulomb attraction between analyte and gold nanoparticle can trigger spontaneous formation of molecule-hotspot pairing with high precision,stability and robustness.The scheme has enabled realization of universal,robust,fast,and large-scale uniform SM-SERS detection for three Raman molecules of rhodamine B,rhodamine 6G,and crystal violet with a very low detection limit of 10−16 M and at a very fast spectrum acquisition time of 50 ms.
基金the National Natural Science Foundation of China(No.12174229 and 22375117)Natural Science Foundation of Shandong Province(No.ZR2022YQ02 and ZR2023MB149)Taishan Scholars Program of Shandong Province(No.tsqn202306152)for financial support.
文摘Quantitative detection of trace small-sized nanoplastics(<100 nm)remains a significant challenge in surface-enhanced Raman scattering(SERS).To tackle this issue,we developed a hydrophobic CuO@Ag nanowire substrate and introduced a multiplex-feature analysis strategy based on the coffee ring effect.This substrate not only offers high Raman enhancement but also exhibits a high probability of detection(POD),enabling rapid and accurate identification of 50 nm polystyrene nanoplastics over a broad concentration range(1–10−10 wt%).Importantly,experimental results reveal a strong correlation between the coffee ring formation and the concentration of nanoplastic dispersion.By incorporating Raman signal intensity,coffee ring diameter,and POD as combined features,we established a machine learning-based mapping between nanoplastic concentration and coffee ring characteristics,allowing precise predictions of dispersion concentration.The mean squared error of these predictions is remarkably low,ranging from 0.21 to 0.54,representing a 19 fold improvement in accuracy compared to traditional linear regression-based methods.This strategy effectively integrates SERS with wettability modification techniques,ensuring high sensitivity and fingerprinting capabilities,while addressing the limitations of Raman signal intensity in accurately reflecting concentration changes at ultra-low levels,providing a new idea for precise SERS measurements of nanoplastics.
