In the field of dual-pulse laser-induced breakdown spectroscopy(DP-LIBS)research,the pursuit of methods for determining pulse intervals and other parameters quickly and conveniently in order to achieve optimal spectra...In the field of dual-pulse laser-induced breakdown spectroscopy(DP-LIBS)research,the pursuit of methods for determining pulse intervals and other parameters quickly and conveniently in order to achieve optimal spectral signal enhancement is paramount.To aid researchers in identification of optimal signal enhancement conditions and more accurate interpretation of the underlying signal enhancement mechanisms,theoretical simulations of the spatiotemporal processes of coaxial DP-LIBS-induced plasma have been established in this work.Using a model based on laser ablation and two-dimensional axisymmetric fluid dynamics,plasma evolutions during aluminum–magnesium alloy laser ablation under single-pulse and coaxial dualpulse excitations have been simulated.The influences of factors,such as delay time,laser fluence,plasma temperature,and particle number density,on the DP-LIBS spectral signals are investigated.Under pulse intervals ranging from 50 to 1500 ns,the time evolutions of spectral line intensity,dual-pulse emission enhancement relative to the single-pulse results,laser irradiance,spatial distribution of plasma temperature and species number density,as well as laser irradiance shielded by plasma have been obtained.The study indicates that the main reason behind the radiation signal enhancement in coaxial DP-LIBS-induced plasma is attributed to the increased species number density and plasma temperature caused by the second laser,and it is inferred that the shielding effect of the plasma mainly occurs in the boundary layer of the stagnation point flow over the target surface.This research provides a theoretical basis for experimental research,parameter optimization,and signal enhancement tracing in DP-LIBS.展开更多
In this paper,a novel four-prong quartz tuning fork(QTF)was designed with enlarged deformation area,large prong gap,and low resonant frequency to improve its performance in laser spectroscopy sensing.A theoretical sim...In this paper,a novel four-prong quartz tuning fork(QTF)was designed with enlarged deformation area,large prong gap,and low resonant frequency to improve its performance in laser spectroscopy sensing.A theoretical simulation model was established to optimize the design of the QTF structure.In the simulation of quartz-enhanced photoacoustic spectroscopy(QEPAS)technology,the maximum stress and the surface charge density of the four-prong QTF demonstrated increases of 11.1-fold and 15.9-fold,respectively,compared to that of the standard two-prong QTF.In the simulation of light-induced thermoelastic spectroscopy(LITES)technology,the surface temperature difference of the four-prong QTF was found to be 11.4 times greater than that of the standard QTF.Experimental results indicated that the C_(2)H_(2)-QEPAS system based on this innovative design improved the signal-to-noise-ratio(SNR)by 4.67 times compared with the standard QTF-based system,and the SNR could increase up to 147.72 times when the four-prong QTF was equipped with its optimal acoustic micro-resonator(AmR).When the average time of the system reached 370 s,the system achieved a MDL as low as 21 ppb.The four-prong QTF-based C_(2)H_(2)-LITES system exhibited a SNR improvement by a factor of 4.52,and a MDL of 96 ppb was obtained when the average time of the system reached 100 s.The theoretical and experimental results effectively demonstrated the superiority of the four-prong QTF in the field of laser spectroscopy sensing.展开更多
Background:Magnetic resonance spectroscopy(MRS)represents a significant advancement in the noninvasive assessment of brain metabolism.MRS can provide valuable metabolic information and facilitate more accurate diagnos...Background:Magnetic resonance spectroscopy(MRS)represents a significant advancement in the noninvasive assessment of brain metabolism.MRS can provide valuable metabolic information and facilitate more accurate diagnoses of intrauterine fetal brain development than was previously possible.To obtain information regarding normal intrauterine fetal brain metabolism and to establish gestational age-specific reference values for normal fetal brain metabolites for subsequent use in MRS,we conducted MRS scans of normal fetal brains during mid-to late-term pregnancies,along with related processing.Methods:In this prospective study,MRS scans were conducted on 109 fetuses,with a total of 54 normal fetal brains enrolled on the basis of specific inclusion and exclusion criteria.We analyzed metabolic ratios,including the sum of N-acetylaspartate(NAA)and total N-acetylaspartate(tNAA),total choline(tCho),inositol(Ins),and total creatine(tCr),in relation to gestational age.Results:Gestational age was significantly correlated with specific metabolic ratios(Ins/tCr:r=-0.75,p<0.0001;tCho/tCr:r=-0.50,p<0.0001),especially tNAA/tCho(tNAA/tCho:r=0.54,p<0.0001)and tNAA/Ins(r=0.56,p<0.0001),providing a baseline for fetal brain metabolic assessment.Linear regression analysis was used to calculate regression lines for fetal brain metabolite ratios.Slopes were tested at p of 0.05.Conclusions:The current findings confirmed a significant correlation between fetal brain metabolites and gestational age,supporting the feasibility of establishing standard values for these metabolites in fetal brain assessment.展开更多
Atmospheric chemistry research and atmospheric measurement techniques have mutually promoted each other and developed rapidly in China in recent years.Cavity-based absorption spectroscopy,which uses a high-finesse cav...Atmospheric chemistry research and atmospheric measurement techniques have mutually promoted each other and developed rapidly in China in recent years.Cavity-based absorption spectroscopy,which uses a high-finesse cavity to achieve very long absorption path-length,thereby achieving ultra-high detection sensitivity,plays an extremely important role in atmospheric chemistry research.Based on the Beer–Lambert law,this technology has the unique advantages of being non-destructive,chemical-free,and highly selective.It does not require any sample preparation and can quantitatively analyze atmospheric trace gases in real time and in situ.In this paper,we review the following:(1)key technological advances in different cavity-based absorption spectroscopy techniques,including cavity ring-down spectroscopy,cavityenhanced absorption spectroscopy,cavity attenuated phase shift spectroscopy,and their extensions;and(2)applications of these techniques in the detection of atmospheric reactive species,such as total peroxy radical,formaldehyde,and reactive nitrogen(e.g.,NOx,HONO,peroxy nitrates,and alkyl nitrates).The review systematically introduces cavity-based absorption spectroscopy techniques and their applications in atmospheric chemistry,which will help promote further communication and cooperation in the fields of laser spectroscopy and atmospheric chemistry.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
In this editorial,we comment on the recent article by Fei et al exploring the field of near-infrared spectroscopy(NIRS)research in schizophrenia from a bibliometrics perspective.In recent years,NIRS has shown unique a...In this editorial,we comment on the recent article by Fei et al exploring the field of near-infrared spectroscopy(NIRS)research in schizophrenia from a bibliometrics perspective.In recent years,NIRS has shown unique advantages in the auxiliary diagnosis of schizophrenia,and the introduction of bibliometrics has provided a macro perspective for research in this field.Despite the opportunities brought about by these technological developments,remaining challenges require multidi-sciplinary approach to devise a reliable and accurate diagnosis system for schizo-phrenia.Nonetheless,NIRS-assisted technology is expected to contribute to the division of methods for early intervention and treatment of schizophrenia.展开更多
In the near-infrared(NIR)spectroscopic data of complex sample systems,such as tobacco leaves,nonlinearity is fairly significant between the absorbance and concentration.This nonlinearity severely degrades the quantita...In the near-infrared(NIR)spectroscopic data of complex sample systems,such as tobacco leaves,nonlinearity is fairly significant between the absorbance and concentration.This nonlinearity severely degrades the quantitative results of traditional methods,such as partial least squares regression(PLS),which can be used to construct linear models.The problem was addressed in this study by using deep learning(DL).We employed three different DL models:a one-dimensional convolutional neural network(1D CNN),a deep neural network(DNN),and a stacked autoencoder with feedforward neural networks(SAE-FNNs).By carefully selecting and tuning the architectures and parameters of these models,we were able to find the most suitable model for dealing with such nonlinear relationships.Our experimental findings reveal that both the DNN and the SAE-FNN models excel in addressing the nonlinear issues of pectin concentration in tobacco,surpassing the performance of the classic linear model(PLS).Specifically,the DNN model stands out for its low average root mean squared error of prediction(RMSEP)value and small standard deviation(SD)of RMSEPs,leading to a tighter and more centered distribution of residuals in the prediction set.These DL models not only proficiently identify complex patterns within NIR data but also boast high prediction accuracy and fast implementation,demonstrating their effectiveness in analytical applications.展开更多
In sub nanometer carbon nanotubes,water exhibits unique dynamic characteristics,and in the high-frequency region of the infrared spectrum,where the stretching vibrations of the internal oxygen-hydrogen(O-H)bonds are c...In sub nanometer carbon nanotubes,water exhibits unique dynamic characteristics,and in the high-frequency region of the infrared spectrum,where the stretching vibrations of the internal oxygen-hydrogen(O-H)bonds are closely related to the hydrogen bonds(H-bonds)network between water molecules.Therefore,it is crucial to analyze the relationship between these two aspects.In this paper,the infrared spectrum and motion characteristics of the stretching vibrations of the O-H bonds in one-dimensional confined water(1DCW)and bulk water(BW)in(6,6)single-walled carbon nanotubes(SWNT)are studied by molecular dynamics simulations.The results show that the stretching vibrations of the two O-H bonds in 1DCW exhibit different frequencies in the infrared spectrum,while the O-H bonds in BW display two identical main frequency peaks.Further analysis using the spring oscillator model reveals that the difference in the stretching amplitude of the O-H bonds is the main factor causing the change in vibration frequency,where an increase in stretching amplitude leads to a decrease in spring stiffness and,consequently,a lower vibration frequency.A more in-depth study found that the interaction of H-bonds between water molecules is the fundamental cause of the increased stretching amplitude and decreased vibration frequency of the O-H bonds.Finally,by analyzing the motion trajectory of the H atoms,the dynamic differences between 1DCW and BW are clearly revealed.These findings provide a new perspective for understanding the behavior of water molecules at the nanoscale and are of significant importance in advancing the development of infrared spectroscopy detection technology.展开更多
All-solid-state lithium batteries(ASSLBs)are strongly considered as the next-generation energy storage devices for their high energy density and intrinsic safety.The solid-solid contact between lithium metal and solid...All-solid-state lithium batteries(ASSLBs)are strongly considered as the next-generation energy storage devices for their high energy density and intrinsic safety.The solid-solid contact between lithium metal and solid electrolyte plays a vital role in the performance of working ASSLBs,which is challenging to investigate quantitatively by experimental approach.This work proposed a quantitative model based on the finite element method for electrochemical impedance spectroscopy simulation of different solid-solid contact states in ASSLBs.With the assistance of an equivalent circuit model and distribution of relaxation times,it is discovered that as the number of voids and the sharpness of cracks increase,the contact resistance Rcgrows and ultimately dominates the battery impedance.Through accurate fitting,inverse proportional relations between contact resistance Rcand(1-porosity)as well as crack angle was disclosed.This contribution affords a fresh insight into clarifying solid-solid contact states in ASSLBs.展开更多
Although there are numerous optical spectroscopy techniques and methods that have been used to extract the fundamental bandgap of a semiconductor,most of them belong to one of these three approaches:(1)the excitonic a...Although there are numerous optical spectroscopy techniques and methods that have been used to extract the fundamental bandgap of a semiconductor,most of them belong to one of these three approaches:(1)the excitonic absorption,(2)modulation spectroscopy,and(3)the most widely used Tauc-plot.The excitonic absorption is based on a many-particle theory,which is physically the most correct approach,but requires more stringent crystalline quality and appropriate sample preparation and experimental implementation.The Tauc-plot is based on a single-particle theo⁃ry that neglects the many-electron effects.Modulation spectroscopy analyzes the spectroscopy features in the derivative spectrum,typically,of the reflectance and transmission under an external perturbation.Empirically,the bandgap ener⁃gy derived from the three approaches follow the order of E_(ex)>E_(MS)>E_(TP),where three transition energies are from exci⁃tonic absorption,modulation spectroscopy,and Tauc-plot,respectively.In principle,defining E_(g) as the single-elec⁃tron bandgap,we expect E_(g)>E_(ex),thus,E_(g)>E_(TP).In the literature,E_(TP) is often interpreted as E_(g),which is conceptual⁃ly problematic.However,in many cases,because the excitonic peaks are not readily identifiable,the inconsistency be⁃tween E_(g) and E_(TP) becomes invisible.In this brief review,real world examples are used(1)to illustrate how excitonic absorption features depend sensitively on the sample and measurement conditions;(2)to demonstrate the differences between E_(ex),E_(MS),and E_(TP) when they can be extracted simultaneously for one sample;and(3)to show how the popular⁃ly adopted Tauc-plot could lead to misleading results.Finally,it is pointed out that if the excitonic absorption is not ob⁃servable,the modulation spectroscopy can often yield a more useful and reasonable bandgap than Tauc-plot.展开更多
This communication looks at the photo-oxidation of polythene and polypropylene plastic bottle tops that are placed on soil in a hot arid environment. The degree of oxidation of the plastic is monitored by FT-IR spectr...This communication looks at the photo-oxidation of polythene and polypropylene plastic bottle tops that are placed on soil in a hot arid environment. The degree of oxidation of the plastic is monitored by FT-IR spectroscopy. It is noted that while different bottle top types photo-oxidize at different rates, all show an appreciable level of oxidation after half a year of exposure to the environment. The oxidation leads to brittleness of the plastic, which leads to fissure formation in bottle tops of little thickness. This leads to fragmentation of the material upon impact, making plastic bottle tops an appreciable source of microplastics.展开更多
To address the issues of peak overlap caused by complex matrices in agricultural product terahertz(THz)spectral signals and the dynamic,nonlinear interference induced by environmental and system noise,this study explo...To address the issues of peak overlap caused by complex matrices in agricultural product terahertz(THz)spectral signals and the dynamic,nonlinear interference induced by environmental and system noise,this study explores the feasibility of adaptive-signal-decomposition-based denoising methods to improve THz spectral quality.THz time-domain spectroscopy(THz-TDS)combined with an attenuated total reflection(ATR)accessory was used to collect THz absorbance spectra from 48 peanut samples.Taking the quantitative prediction model of peanut moisture content based on THz-ATR as an example,wavelet transform(WT),empirical mode decomposition(EMD),local mean decomposition(LMD),and its improved methods-segmented local mean decomposition(SLMD)and piecewise mirror extension local mean decomposition(PME-LMD)-were employed for spectral denoising.The applicability of different denoising methods was evaluated using a support vector regression(SVR)model.Experimental results show that the peanut moisture content prediction model constructed after PME-LMD denoising achieved the best performance,with a root mean square error(RMSE),coefficient of determination(R^(2)),and mean absolute percentage error(MAPE)of 0.010,0.912,and 0.040,respectively.Compared with traditional methods,PME-LMD significantly improved spectral quality and model prediction performance.The PME-LMD denoising strategy proposed in this study effectively suppresses non-uniform noise interference in THz spectral signals,providing an efficient and accurate preprocessing method for THz spectral analysis of agricultural products.This research provides theoretical support and technical guidance for the application of THz technology for detecting agricultural product quality.展开更多
Antifungal resistance is the leading cause of antifungal treatment failure in invasive candidiasis.Metabolic rewiring could become a new insight to account for antifungal resistance as to find innovative clinical ther...Antifungal resistance is the leading cause of antifungal treatment failure in invasive candidiasis.Metabolic rewiring could become a new insight to account for antifungal resistance as to find innovative clinical therapies.Here,we show that dynamic surface-enhanced Raman spectroscopy is a promising tool to identify the metabolic differences between fluconazole(Diflucan)-resistant and fluconazole(Diflucan)-sensitive Candida albicans through the signatures of biochemical components and complemented with machine learning algorithms and two-dimensional correlation spectroscopy,an underlying resistance mechanism,that is,the change of purine metabolites induced the resistance of Candida albicans has been clarified yet never reported anywhere.We hope the integrated methodology introduced in this work could be beneficial for the interpretation of cellular regulation,propelling the development of targeted antifungal therapies and diagnostic tools for more efficient management of severe antifungal resistance.展开更多
Revealing the factors that affect the vibrational frequency of Stark probe at interface is a pre-requirement for evaluating the absolute interfacial electric field.Here using surface-enhanced infrared absorption(SEIRA...Revealing the factors that affect the vibrational frequency of Stark probe at interface is a pre-requirement for evaluating the absolute interfacial electric field.Here using surface-enhanced infrared absorption(SEIRA)spectroscopy,attenuated total reflection(ATR)spectroscopy and molecular dynamics(MD),we reveal the assembled C≡N at gold nanofilm exhibits a reduced Stark tuning rate(STR)referring to the vibrational frequency shift in response to electric field comparing with the bulk which was regulated by the electron transfer between S and Au.These findings lead to a deeper understanding of the vibrational Stark effect at the interface and provide guidance for improving the interface electric field theory.展开更多
Infrared(IR)spectroscopy,a technique within the realm of molecular vibrational spectroscopy,furnishes distinctive chemical signatures pivotal for both structural analysis and compound identification.A notable challeng...Infrared(IR)spectroscopy,a technique within the realm of molecular vibrational spectroscopy,furnishes distinctive chemical signatures pivotal for both structural analysis and compound identification.A notable challenge emerges from the misalignment between the mid-IR light wavelength range and molecular dimensions,culminating in a constrained absorption cross-section and diminished vibrational absorption coefficients(Supplementary data).展开更多
We present a comprehensive investigation of the vibrational spectra and conformational distribution of neutral and cationic monoethanolamine(MEA)in the gas phase.Using infrared-vacuum ultraviolet non-resonant ionizati...We present a comprehensive investigation of the vibrational spectra and conformational distribution of neutral and cationic monoethanolamine(MEA)in the gas phase.Using infrared-vacuum ultraviolet non-resonant ionization fragmentation detected IR spectroscopy(NRIFD-IR),we obtained vibrational spectra in the 2500-3800 cm^(−1)range for both neutral and cationic MEA.Density functional theory(DFT)calculations at the B3LYPD3(BJ)/def2-TZVPP level were employed to elucidate the molecular structures and vibrational modes.Our analysis revealed twelve distinct conformers for neutral MEA,with N1gʹGgʹbeing the most stable,while cationic MEA exhibited four conformers,among which C1gʹGt conformer was found to be the primary contributor to the observed spectra.The experimental spectra were interpreted through comparison with anharmonic calculations,allowing for detailed assignment of vibrational modes.Notably,we observed significant differences in the OH stretch region between neutral and cationic species,reflecting changes in intramolecular hydrogen bonding upon ionization.Furthermore,our study highlights the necessity for distinct scaling factors when calculating harmonic frequencies for neutral and cationic substances.展开更多
Objective The national lifetime prevalence of urolithiasis is estimated at 6.6%in Iran.However,reports on the composition of kidney stones have been based on imprecise methods like the chemical analysis.No prior large...Objective The national lifetime prevalence of urolithiasis is estimated at 6.6%in Iran.However,reports on the composition of kidney stones have been based on imprecise methods like the chemical analysis.No prior large-scale study has reported the composition of kidney stones based on the gold-standard methods(X-ray diffraction or infrared spectroscopy)in Iran.This study aimed to provide the composition of kidney stones based on Fourier transform infrared spectroscopy.Methods This is a cross-sectional study assessing urinary stone composition from various cities in Iran at a referral center using infrared spectroscopy from February 2019 to March 2023.Results This study determined the stone composition of 1092 patients from 10 cities in Iran.Overall,the majority of stones were composed of calcium oxalate(n=498;45.6%)and uric acid(UA,n=488;44.7%)followed by cystine(n=49;4.5%)and struvite(n=28;2.6%).Stone composition in Shiraz and Isfahan was roughly similar with a higher percentage of UA stones(53.4%and 53.6%,respectively)while the capital city of Iran(Tehran)had less frequent UA stones(39.9%)with a higher percentage of calcium oxalate stones.The percentage of UA stones increased with age as it was 11.1%in children,42.7%in adults,and 83.3%in geriatric patients(p<0.001).About 29.6%of cystine stones were observed in children.Conclusion The most frequent stone composition among kidney stones in Iran was calcium oxalate and UA stones.This relative frequency of UA stones is considerably higher than many international reports from neighboring as well as distant countries.More cystine stones were observed in children and women.Geriatric patients’stones were mostly composed of UA.展开更多
基金supported by the National Key R&D Program of China (No. 2017YFA0304203)the National Energy R&D Center of Petroleum Refining Technology (RIPP, SINOPEC)+3 种基金Changjiang Scholars and Innovative Research Team at the University of the Ministry of Education of China (No. IRT_17R70)National Natural Science Foundation of China (NSFC) (Nos. 61975103, 61875108 and 627010407)111 Project (No. D18001)Fund for Shanxi (No. 1331KSC)
文摘In the field of dual-pulse laser-induced breakdown spectroscopy(DP-LIBS)research,the pursuit of methods for determining pulse intervals and other parameters quickly and conveniently in order to achieve optimal spectral signal enhancement is paramount.To aid researchers in identification of optimal signal enhancement conditions and more accurate interpretation of the underlying signal enhancement mechanisms,theoretical simulations of the spatiotemporal processes of coaxial DP-LIBS-induced plasma have been established in this work.Using a model based on laser ablation and two-dimensional axisymmetric fluid dynamics,plasma evolutions during aluminum–magnesium alloy laser ablation under single-pulse and coaxial dualpulse excitations have been simulated.The influences of factors,such as delay time,laser fluence,plasma temperature,and particle number density,on the DP-LIBS spectral signals are investigated.Under pulse intervals ranging from 50 to 1500 ns,the time evolutions of spectral line intensity,dual-pulse emission enhancement relative to the single-pulse results,laser irradiance,spatial distribution of plasma temperature and species number density,as well as laser irradiance shielded by plasma have been obtained.The study indicates that the main reason behind the radiation signal enhancement in coaxial DP-LIBS-induced plasma is attributed to the increased species number density and plasma temperature caused by the second laser,and it is inferred that the shielding effect of the plasma mainly occurs in the boundary layer of the stagnation point flow over the target surface.This research provides a theoretical basis for experimental research,parameter optimization,and signal enhancement tracing in DP-LIBS.
基金supports from the National Natural Science Foundation of China(Grant Nos.62335006,62022032,62275065,and 62405078)Key Laboratory of Opto-Electronic Information Acquisition and Manipulation(Anhui University),Ministry of Education(Grant No.OEIAM202202)+2 种基金Fundamental Research Funds for the Central Universities(Grant No.HIT.OCEF.2023011)China Postdoctoral Science Foundation(Grant No.2024M764172)Heilongjiang Postdoctoral Fund(Grant No.LBH-Z23144).
文摘In this paper,a novel four-prong quartz tuning fork(QTF)was designed with enlarged deformation area,large prong gap,and low resonant frequency to improve its performance in laser spectroscopy sensing.A theoretical simulation model was established to optimize the design of the QTF structure.In the simulation of quartz-enhanced photoacoustic spectroscopy(QEPAS)technology,the maximum stress and the surface charge density of the four-prong QTF demonstrated increases of 11.1-fold and 15.9-fold,respectively,compared to that of the standard two-prong QTF.In the simulation of light-induced thermoelastic spectroscopy(LITES)technology,the surface temperature difference of the four-prong QTF was found to be 11.4 times greater than that of the standard QTF.Experimental results indicated that the C_(2)H_(2)-QEPAS system based on this innovative design improved the signal-to-noise-ratio(SNR)by 4.67 times compared with the standard QTF-based system,and the SNR could increase up to 147.72 times when the four-prong QTF was equipped with its optimal acoustic micro-resonator(AmR).When the average time of the system reached 370 s,the system achieved a MDL as low as 21 ppb.The four-prong QTF-based C_(2)H_(2)-LITES system exhibited a SNR improvement by a factor of 4.52,and a MDL of 96 ppb was obtained when the average time of the system reached 100 s.The theoretical and experimental results effectively demonstrated the superiority of the four-prong QTF in the field of laser spectroscopy sensing.
基金supported by China Society for Maternal and Child Health Research(Gant/Award Number:2023CAMCHS003A17).
文摘Background:Magnetic resonance spectroscopy(MRS)represents a significant advancement in the noninvasive assessment of brain metabolism.MRS can provide valuable metabolic information and facilitate more accurate diagnoses of intrauterine fetal brain development than was previously possible.To obtain information regarding normal intrauterine fetal brain metabolism and to establish gestational age-specific reference values for normal fetal brain metabolites for subsequent use in MRS,we conducted MRS scans of normal fetal brains during mid-to late-term pregnancies,along with related processing.Methods:In this prospective study,MRS scans were conducted on 109 fetuses,with a total of 54 normal fetal brains enrolled on the basis of specific inclusion and exclusion criteria.We analyzed metabolic ratios,including the sum of N-acetylaspartate(NAA)and total N-acetylaspartate(tNAA),total choline(tCho),inositol(Ins),and total creatine(tCr),in relation to gestational age.Results:Gestational age was significantly correlated with specific metabolic ratios(Ins/tCr:r=-0.75,p<0.0001;tCho/tCr:r=-0.50,p<0.0001),especially tNAA/tCho(tNAA/tCho:r=0.54,p<0.0001)and tNAA/Ins(r=0.56,p<0.0001),providing a baseline for fetal brain metabolic assessment.Linear regression analysis was used to calculate regression lines for fetal brain metabolite ratios.Slopes were tested at p of 0.05.Conclusions:The current findings confirmed a significant correlation between fetal brain metabolites and gestational age,supporting the feasibility of establishing standard values for these metabolites in fetal brain assessment.
基金supported by the National Natural Science Foundation of China(Grant Nos.U21A2028,42022051,62275250,42030609,41627810,91644107,and 91544228).
文摘Atmospheric chemistry research and atmospheric measurement techniques have mutually promoted each other and developed rapidly in China in recent years.Cavity-based absorption spectroscopy,which uses a high-finesse cavity to achieve very long absorption path-length,thereby achieving ultra-high detection sensitivity,plays an extremely important role in atmospheric chemistry research.Based on the Beer–Lambert law,this technology has the unique advantages of being non-destructive,chemical-free,and highly selective.It does not require any sample preparation and can quantitatively analyze atmospheric trace gases in real time and in situ.In this paper,we review the following:(1)key technological advances in different cavity-based absorption spectroscopy techniques,including cavity ring-down spectroscopy,cavityenhanced absorption spectroscopy,cavity attenuated phase shift spectroscopy,and their extensions;and(2)applications of these techniques in the detection of atmospheric reactive species,such as total peroxy radical,formaldehyde,and reactive nitrogen(e.g.,NOx,HONO,peroxy nitrates,and alkyl nitrates).The review systematically introduces cavity-based absorption spectroscopy techniques and their applications in atmospheric chemistry,which will help promote further communication and cooperation in the fields of laser spectroscopy and atmospheric chemistry.
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.
文摘In this editorial,we comment on the recent article by Fei et al exploring the field of near-infrared spectroscopy(NIRS)research in schizophrenia from a bibliometrics perspective.In recent years,NIRS has shown unique advantages in the auxiliary diagnosis of schizophrenia,and the introduction of bibliometrics has provided a macro perspective for research in this field.Despite the opportunities brought about by these technological developments,remaining challenges require multidi-sciplinary approach to devise a reliable and accurate diagnosis system for schizo-phrenia.Nonetheless,NIRS-assisted technology is expected to contribute to the division of methods for early intervention and treatment of schizophrenia.
基金supported by a joint project with SINOPEC(Dalian)Research Institute of Petroleum and Petrochemicals Co.,Ltd.(Contract No.323061).
文摘In the near-infrared(NIR)spectroscopic data of complex sample systems,such as tobacco leaves,nonlinearity is fairly significant between the absorbance and concentration.This nonlinearity severely degrades the quantitative results of traditional methods,such as partial least squares regression(PLS),which can be used to construct linear models.The problem was addressed in this study by using deep learning(DL).We employed three different DL models:a one-dimensional convolutional neural network(1D CNN),a deep neural network(DNN),and a stacked autoencoder with feedforward neural networks(SAE-FNNs).By carefully selecting and tuning the architectures and parameters of these models,we were able to find the most suitable model for dealing with such nonlinear relationships.Our experimental findings reveal that both the DNN and the SAE-FNN models excel in addressing the nonlinear issues of pectin concentration in tobacco,surpassing the performance of the classic linear model(PLS).Specifically,the DNN model stands out for its low average root mean squared error of prediction(RMSEP)value and small standard deviation(SD)of RMSEPs,leading to a tighter and more centered distribution of residuals in the prediction set.These DL models not only proficiently identify complex patterns within NIR data but also boast high prediction accuracy and fast implementation,demonstrating their effectiveness in analytical applications.
基金Supported by the Natural Science Foundation of China(51705326,52075339)。
文摘In sub nanometer carbon nanotubes,water exhibits unique dynamic characteristics,and in the high-frequency region of the infrared spectrum,where the stretching vibrations of the internal oxygen-hydrogen(O-H)bonds are closely related to the hydrogen bonds(H-bonds)network between water molecules.Therefore,it is crucial to analyze the relationship between these two aspects.In this paper,the infrared spectrum and motion characteristics of the stretching vibrations of the O-H bonds in one-dimensional confined water(1DCW)and bulk water(BW)in(6,6)single-walled carbon nanotubes(SWNT)are studied by molecular dynamics simulations.The results show that the stretching vibrations of the two O-H bonds in 1DCW exhibit different frequencies in the infrared spectrum,while the O-H bonds in BW display two identical main frequency peaks.Further analysis using the spring oscillator model reveals that the difference in the stretching amplitude of the O-H bonds is the main factor causing the change in vibration frequency,where an increase in stretching amplitude leads to a decrease in spring stiffness and,consequently,a lower vibration frequency.A more in-depth study found that the interaction of H-bonds between water molecules is the fundamental cause of the increased stretching amplitude and decreased vibration frequency of the O-H bonds.Finally,by analyzing the motion trajectory of the H atoms,the dynamic differences between 1DCW and BW are clearly revealed.These findings provide a new perspective for understanding the behavior of water molecules at the nanoscale and are of significant importance in advancing the development of infrared spectroscopy detection technology.
基金supported by the Beijing Natural Science Foundation(Z200011,L233004)the National Key Research and Development Program(2021YFB2500300)+3 种基金the National Natural Science Foundation of China(52394170,52394171,22109011,22393900,and 22108151)the Tsinghua-Jiangyin Innovation Special Fund(TJISF)(2022JYTH0101)the S&T Program of Hebei(22344402D)the Tsinghua University Initiative Scientific Research Program.
文摘All-solid-state lithium batteries(ASSLBs)are strongly considered as the next-generation energy storage devices for their high energy density and intrinsic safety.The solid-solid contact between lithium metal and solid electrolyte plays a vital role in the performance of working ASSLBs,which is challenging to investigate quantitatively by experimental approach.This work proposed a quantitative model based on the finite element method for electrochemical impedance spectroscopy simulation of different solid-solid contact states in ASSLBs.With the assistance of an equivalent circuit model and distribution of relaxation times,it is discovered that as the number of voids and the sharpness of cracks increase,the contact resistance Rcgrows and ultimately dominates the battery impedance.Through accurate fitting,inverse proportional relations between contact resistance Rcand(1-porosity)as well as crack angle was disclosed.This contribution affords a fresh insight into clarifying solid-solid contact states in ASSLBs.
基金Supported by Bissell Distinguished Professor Endowment Fund at UNC-Charlotte。
文摘Although there are numerous optical spectroscopy techniques and methods that have been used to extract the fundamental bandgap of a semiconductor,most of them belong to one of these three approaches:(1)the excitonic absorption,(2)modulation spectroscopy,and(3)the most widely used Tauc-plot.The excitonic absorption is based on a many-particle theory,which is physically the most correct approach,but requires more stringent crystalline quality and appropriate sample preparation and experimental implementation.The Tauc-plot is based on a single-particle theo⁃ry that neglects the many-electron effects.Modulation spectroscopy analyzes the spectroscopy features in the derivative spectrum,typically,of the reflectance and transmission under an external perturbation.Empirically,the bandgap ener⁃gy derived from the three approaches follow the order of E_(ex)>E_(MS)>E_(TP),where three transition energies are from exci⁃tonic absorption,modulation spectroscopy,and Tauc-plot,respectively.In principle,defining E_(g) as the single-elec⁃tron bandgap,we expect E_(g)>E_(ex),thus,E_(g)>E_(TP).In the literature,E_(TP) is often interpreted as E_(g),which is conceptual⁃ly problematic.However,in many cases,because the excitonic peaks are not readily identifiable,the inconsistency be⁃tween E_(g) and E_(TP) becomes invisible.In this brief review,real world examples are used(1)to illustrate how excitonic absorption features depend sensitively on the sample and measurement conditions;(2)to demonstrate the differences between E_(ex),E_(MS),and E_(TP) when they can be extracted simultaneously for one sample;and(3)to show how the popular⁃ly adopted Tauc-plot could lead to misleading results.Finally,it is pointed out that if the excitonic absorption is not ob⁃servable,the modulation spectroscopy can often yield a more useful and reasonable bandgap than Tauc-plot.
文摘This communication looks at the photo-oxidation of polythene and polypropylene plastic bottle tops that are placed on soil in a hot arid environment. The degree of oxidation of the plastic is monitored by FT-IR spectroscopy. It is noted that while different bottle top types photo-oxidize at different rates, all show an appreciable level of oxidation after half a year of exposure to the environment. The oxidation leads to brittleness of the plastic, which leads to fissure formation in bottle tops of little thickness. This leads to fragmentation of the material upon impact, making plastic bottle tops an appreciable source of microplastics.
基金Supported by the National Key R&D Program of China(2023YFD2101001)National Natural Science Foundation of China(32202144,61807001)。
文摘To address the issues of peak overlap caused by complex matrices in agricultural product terahertz(THz)spectral signals and the dynamic,nonlinear interference induced by environmental and system noise,this study explores the feasibility of adaptive-signal-decomposition-based denoising methods to improve THz spectral quality.THz time-domain spectroscopy(THz-TDS)combined with an attenuated total reflection(ATR)accessory was used to collect THz absorbance spectra from 48 peanut samples.Taking the quantitative prediction model of peanut moisture content based on THz-ATR as an example,wavelet transform(WT),empirical mode decomposition(EMD),local mean decomposition(LMD),and its improved methods-segmented local mean decomposition(SLMD)and piecewise mirror extension local mean decomposition(PME-LMD)-were employed for spectral denoising.The applicability of different denoising methods was evaluated using a support vector regression(SVR)model.Experimental results show that the peanut moisture content prediction model constructed after PME-LMD denoising achieved the best performance,with a root mean square error(RMSE),coefficient of determination(R^(2)),and mean absolute percentage error(MAPE)of 0.010,0.912,and 0.040,respectively.Compared with traditional methods,PME-LMD significantly improved spectral quality and model prediction performance.The PME-LMD denoising strategy proposed in this study effectively suppresses non-uniform noise interference in THz spectral signals,providing an efficient and accurate preprocessing method for THz spectral analysis of agricultural products.This research provides theoretical support and technical guidance for the application of THz technology for detecting agricultural product quality.
基金supported by grants from the National Natural Science Foundation of China(Nos.22074015 and 82074428)Youth Talent Cultivation Initiation Fund of Zhongda Hospital,Southeast University(No.CZXM-GSP-RC110)to Hao Li+1 种基金Evidence-Based Capacity Building for TCM Specialty Therapies for Skin Diseases of National Administration of TCMInnovative Team Projects of Shanghai Municipal Commission of Health(No.2022CX011)to Fulun Li.
文摘Antifungal resistance is the leading cause of antifungal treatment failure in invasive candidiasis.Metabolic rewiring could become a new insight to account for antifungal resistance as to find innovative clinical therapies.Here,we show that dynamic surface-enhanced Raman spectroscopy is a promising tool to identify the metabolic differences between fluconazole(Diflucan)-resistant and fluconazole(Diflucan)-sensitive Candida albicans through the signatures of biochemical components and complemented with machine learning algorithms and two-dimensional correlation spectroscopy,an underlying resistance mechanism,that is,the change of purine metabolites induced the resistance of Candida albicans has been clarified yet never reported anywhere.We hope the integrated methodology introduced in this work could be beneficial for the interpretation of cellular regulation,propelling the development of targeted antifungal therapies and diagnostic tools for more efficient management of severe antifungal resistance.
基金The National Key R&D Program of China(No.2022YFE0113000)the National Science Fund for Distinguished Young Scholars(No.22025406)+1 种基金the National Natural Science Foundation of China(Nos.22074138,12174457)the Youth Innovation Promotion Association of CAS(No.2020233)for financial support。
文摘Revealing the factors that affect the vibrational frequency of Stark probe at interface is a pre-requirement for evaluating the absolute interfacial electric field.Here using surface-enhanced infrared absorption(SEIRA)spectroscopy,attenuated total reflection(ATR)spectroscopy and molecular dynamics(MD),we reveal the assembled C≡N at gold nanofilm exhibits a reduced Stark tuning rate(STR)referring to the vibrational frequency shift in response to electric field comparing with the bulk which was regulated by the electron transfer between S and Au.These findings lead to a deeper understanding of the vibrational Stark effect at the interface and provide guidance for improving the interface electric field theory.
基金supported by National Natural Science Foundation of China(Grant No.:32301161)the Natural Scientific Foundation of Hunan Province,China(Grant No.:2023JJ60052)+3 种基金the Scientific Research Project of Hunan Provincial Health Commission,China(Grant No.:202112062218,20190161)the Scientific Research Project of Hunan Provincial Department of Education,China(Grant No.:22B0455)the Clinical“4310”Project of the University of South China,China(Grant No.:20224310NHYCG02)the Doctoral Scientific Research Foundation of University of South China,China(Grant No.:200XQD042).
文摘Infrared(IR)spectroscopy,a technique within the realm of molecular vibrational spectroscopy,furnishes distinctive chemical signatures pivotal for both structural analysis and compound identification.A notable challenge emerges from the misalignment between the mid-IR light wavelength range and molecular dimensions,culminating in a constrained absorption cross-section and diminished vibrational absorption coefficients(Supplementary data).
基金the Dalian Coherent Light Source (DCLS) for support and assistancesurported by the National Natural Science Foundation of China (No.22288201)+1 种基金the Chinese Academy of Sciences (GJJSTD20220001)the Innovation Program for Quantum Science and Technology (No.2021ZD0303305)。
文摘We present a comprehensive investigation of the vibrational spectra and conformational distribution of neutral and cationic monoethanolamine(MEA)in the gas phase.Using infrared-vacuum ultraviolet non-resonant ionization fragmentation detected IR spectroscopy(NRIFD-IR),we obtained vibrational spectra in the 2500-3800 cm^(−1)range for both neutral and cationic MEA.Density functional theory(DFT)calculations at the B3LYPD3(BJ)/def2-TZVPP level were employed to elucidate the molecular structures and vibrational modes.Our analysis revealed twelve distinct conformers for neutral MEA,with N1gʹGgʹbeing the most stable,while cationic MEA exhibited four conformers,among which C1gʹGt conformer was found to be the primary contributor to the observed spectra.The experimental spectra were interpreted through comparison with anharmonic calculations,allowing for detailed assignment of vibrational modes.Notably,we observed significant differences in the OH stretch region between neutral and cationic species,reflecting changes in intramolecular hydrogen bonding upon ionization.Furthermore,our study highlights the necessity for distinct scaling factors when calculating harmonic frequencies for neutral and cationic substances.
文摘Objective The national lifetime prevalence of urolithiasis is estimated at 6.6%in Iran.However,reports on the composition of kidney stones have been based on imprecise methods like the chemical analysis.No prior large-scale study has reported the composition of kidney stones based on the gold-standard methods(X-ray diffraction or infrared spectroscopy)in Iran.This study aimed to provide the composition of kidney stones based on Fourier transform infrared spectroscopy.Methods This is a cross-sectional study assessing urinary stone composition from various cities in Iran at a referral center using infrared spectroscopy from February 2019 to March 2023.Results This study determined the stone composition of 1092 patients from 10 cities in Iran.Overall,the majority of stones were composed of calcium oxalate(n=498;45.6%)and uric acid(UA,n=488;44.7%)followed by cystine(n=49;4.5%)and struvite(n=28;2.6%).Stone composition in Shiraz and Isfahan was roughly similar with a higher percentage of UA stones(53.4%and 53.6%,respectively)while the capital city of Iran(Tehran)had less frequent UA stones(39.9%)with a higher percentage of calcium oxalate stones.The percentage of UA stones increased with age as it was 11.1%in children,42.7%in adults,and 83.3%in geriatric patients(p<0.001).About 29.6%of cystine stones were observed in children.Conclusion The most frequent stone composition among kidney stones in Iran was calcium oxalate and UA stones.This relative frequency of UA stones is considerably higher than many international reports from neighboring as well as distant countries.More cystine stones were observed in children and women.Geriatric patients’stones were mostly composed of UA.
