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Nanoparticle enhanced laser ablation and consequent effects on laser induced plasma optical emission
摘要： In this paper the plasmon enhanced ablation for elemental analysis is investigated with several experiments in order to point out the crucial questions concerning the laser matter interaction under the effect of plasmonic coupling between the nanoparticle (NP) system and the laser ablation pulse. The correlation between the electromagnetic field enhancement and the signal enhancement during NP enhanced laser induced breakdown spectroscopy (NELIBS), as well as the laser matter interaction at the nanoscale, is discussed in the case of noble metal NPs deposited on metal samples. The results suggest that, while laser pulse energy is concentrated in the space between the NPs, the NP system is shielded by the field enhancement distribution after the laser pulse interacts with the plasmons of the NP system. Finally the comparison of the laser energy transfer to the sample between NELIBS and conventional LIBS is discussed.
关键词： LIBS,Nanoparticle enhanced laser induced breakdown spectroscopy (NELIBS),laser ablation,plasmonic enhanced ablation,LA-ICP-MS
更新于2025-09-23 15:19:57
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An image features assisted line selection method in laser-induced breakdown spectroscopy
摘要： Analytical lines play a crucial role in laser-induced breakdown spectroscopy (LIBS) technology. To improve the classification performance of LIBS, an image features assisted line selection (IFALS) method which based on spectral morphology and the characteristics of Harris corners was proposed. With this method, a classification experiment for 24 metamorphic rock samples was conducted with linear discriminant analysis (LDA) algorithm. The result showed that the classification accuracy was increased from 94.38% of the conventional classification model MLS-LDA (Manual line selection-linear discriminant analysis) to 98.54% of IFALS-LDA. Furthermore, the time required for the whole classification process was decreased from 2768.38 seconds of MLS-LDA to 4.36 seconds of the proposed method, thus the classification efficiency was greatly improved. In addition, compared with the existing automatic line selection method, the convergence rate of IFALS-LDA is significantly faster than that of ASPI (Automatic Spectral Peaks Identification)-LDA. This study demonstrates that LIBS assisted with the image features in machine vision can promote the analytical performance of LIBS technology.
关键词： Laser-induced breakdown spectroscopy,metamorphic rock,image features,linear discrimination analysis,analytical line selection
更新于2025-09-23 15:19:57
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Optimization of Measuring Parameters for Two-dimensional Elemental Mapping in Laser-induced Breakdown Optical Emission Spectrometry Using 1-kHz Q-switched Nd:YAG Laser
摘要： This paper described how the lateral resolution of an elemental mapping was estimated in laser-induced breakdown optical emission spectrometry (LIBS), when the focus point of a high-frequency Q-switched Nd:YAG laser was moved on a sample surface, along with measuring the emission signal from the resultant plasma. Several measuring parameters were optimized to improve the lateral resolution; namely, they were an averaged laser power of 1 mJ/pulse, a laser repetition frequency of 1 kHz, a scanning rate of the laser beam of 0.5 mm/s, and an atmospheric gas pressure of He 1 000 Pa. Using these optimal parameters, a lateral resolution was obtained to be ca. 20 μm in the one-dimensional direction of laser scan. Furthermore, two model samples, in which regularly-aligned copper circles were deposited on a nickel plate, were irradiated by a scanning laser beam to determine actual resolving abilities both in a line direction along travelling the laser and in a two-dimensional direction over a certain sample area. The sample having an interval of 85 μm between the copper circles could give an emission image which was appropriately resolved in the two-dimensional as well as the one-dimensional direction; however, in the other sample having the 25-μm interval, the two-dimensional resolution became degraded compared to the resolution of the line scan, probably because the ablation grooves, which were left on the sample surface, had a width of more than 100 μm and were overlapped with each other in the observed area.
关键词： lateral resolution,copper,scanning laser beam,laser-induced breakdown plasma spectrometry,laser ablation
更新于2025-09-23 15:19:57
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Fast Classification of Geographical Origins of Honey Based on Laser-Induced Breakdown Spectroscopy and Multivariate Analysis
摘要： Traceability of honey is highly required by consumers and food administration with the consideration of food safety and quality. In this study, a technique named laser-induced breakdown spectroscopy (LIBS) was used to fast trace geographical origins of acacia honey and multi-floral honey. LIBS emissions from elements of Mg, Ca, Na, and K had significant differences among different geographical origins. The clusters of honey from different geographical origins were visualized with principal component analysis. In addition, support vector machine (SVM) and linear discrimination analysis (LDA) were used to quantitively classify the origins. The results indicated that SVM performed better than LDA, and the discriminant results of multi-floral honey were better than acacia honey. The accuracy and mean average precision for multi-floral honey were 99.7% and 99.7%, respectively. This study provided a fast approach for geographical origin classification, and might be helpful for food traceability.
关键词： geographical origin,classification,honey,laser-induced breakdown spectroscopy,multivariate analysis
更新于2025-09-23 15:19:57
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Laser-induced breakdown spectroscopy of uranium in the VUV range
摘要： Quantitative analysis of impurities in nuclear materials is necessary in a number of areas, including process control during manufacturing, quality control of products, or for nuclear forensics purposes. Due to the important handling constraints induced by the samples radioactivity and their containment inside airtight enclosures, optical analytical techniques have great advantages over standard ones that require sample preparation, like ICP-based techniques. Therefore, laser-induced breakdown spectroscopy (LIBS) is developed for fast quantitative analysis of impurities in uranium. Actinides are well-known to have a very large number of emission lines in the UV-visible spectral range, hence making the detection of trace or minor elements a real challenge. Therefore, in this study we explored the vacuum ultraviolet range (VUV), i.e. below 200 nm, in order to investigate if this spectral region is more favorable for elemental analysis of uranium by LIBS. As practically no data on VUV spectroscopy of uranium are available, we first analyzed the spectra obtained to assess the spectral density of uranium lines, both in the UV and VUV. Then, the detection limits of two elements, carbon and vanadium, were estimated. It was found that, in spite of a less dense and less intense uranium background in the VUV, this spectral region is not relevant for metal impurities whose spectra are marginally analytically useful in the VUV. Conversely, for non-metals having intense lines in the VUV, the detection limit can be significantly better than in the UV. This was already known for non-nuclear samples. This study extends that conclusion to nuclear materials and has important practical consequences on the implementation of a LIBS analyzer in a nuclear facility.
关键词： vanadium,uranium,Laser-induced breakdown spectroscopy,impurities detection,carbon,VUV range
更新于2025-09-23 15:19:57
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Quantification of calcium in infant formula using laser-induced breakdown spectroscopy (LIBS), Fourier transform mid-infrared (FT-IR) and Raman spectroscopy combined with chemometrics including data fusion
摘要： Laser-induced breakdown spectroscopy (LIBS), Fourier transform mid-infrared (FT-IR) and Raman spectroscopy combined with chemometrics were investigated to quantify calcium (Ca) content in infant formula powder (INF). INF samples (n=51) with calcium content levels (ca. 6.5-30 mg Ca/100kJ) were prepared in accordance with the guidelines of Commission Directive 2006/125/EC. Atomic absorption spectroscopy (AAS) was used as the reference method for Ca content determination. To predict Ca content in INF samples, partial least squares regression (PLSR) models that developed based on LIBS, Raman and FT-IR spectral data, respectively. The model developed using LIBS data achieved the best performance for the quantification of Ca content in INF (R2 (cross-validation (CV))-0.99, RMSECV-0.29 mg/g; R2 (prediction (P))-1, RMSEP-0.63 mg/g). PLSR models that developed based on data fusion of Raman and FT-IR spectral features obtained the second best performance (R2CV-0.97, RMSECV-0.38 mg/g; R2P-0.97, RMSEP-0.36 mg/g). This study demonstrated the potential of LIBS, FT-IR and Raman spectroscopy to accurately quantify Ca content in INF.
关键词： Fourier transform mid-infrared,laser-induced breakdown spectroscopy,chemometrics,Raman spectroscopy,calcium,infant formula
更新于2025-09-23 15:19:57
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Laser ablation at high repetition rate coupled to laser-induced breakdown spectroscopy for analysis of non-matrix matched standards
摘要： Laser ablation at kilohertz repetition rate coupled to laser-induced breakdown spectroscopy (kHz LA-LIBS) was used for the analysis of non-matrix matched metallic standards. Kilohertz LA-LIBS exploited the demonstrated advantages of the analytical technique referred to as laser-ablation laser-induced breakdown spectroscopy (LA-LIBS), while at the same time increased the amount of ablated mass available for analysis. By separating the laser ablation process from the excitation and analysis stages, every configuration of LA-LIBS has demonstrated to produce better analytical results during the analysis of non-matrix matched samples. This research reports the analytical response of five analytes (Al, Cu, Fe, Mg and Mn) from eight standard reference materials. The standards included four aluminum alloys, a high temperature alloy, a cupro-nickel alloy, a stainless steel and a low alloy steel. The analytical performance of kHz LA-LIBS was evaluated through the estimation of the signal-to-noise ratio, relative standard deviation, linearity and y-intercept of calibration curves and limits of detection. Calibration plots relating the analyte concentration to the Fe-normalized (internal standard), peak-to-background and net intensities were constructed. The increased amount of ablated mass in kHz-LA-LIBS rendered superior figures compared with traditional LIBS and other LA-LIBS configurations. The limits of detection of kHz LA-LIBS were improved by 3 to 14 times as compared to those reported previously and were estimated in the range of 0.07 and 0.30% by mass.
关键词： matrix effects,non-matrix matched standards,laser ablation laser-induced breakdown spectroscopy,high repetition laser ablation
更新于2025-09-23 15:19:57
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High-accuracy prediction of carbon content in semi-coke by laser-induced breakdown spectroscopy
摘要： Semi-coke, as one kind of special coal resource with relatively high concentration carbon and low volatility, plays an important role in the coal chemical industry and city clean. Laser-Induced Breakdown Spectroscopy (LIBS) has been proved as an effective way to make an online analysis for the coal products. However, the lower volatility of semi-coke makes it hard to be pressed into a slice to get a smooth surface for a uniform laser-irradiation. Therefore, it is necessary to find an effective way to realize a high-accuracy LIBS detection for semi-coke application. Herein, two feasible ways of sample preparation are tried, one easy way is directly painting semi-coke powders on a tape that suitable for online fast monitoring, and the other complicated way is to mix binder into the semi-coke powder then that the uniformly and tightly coal slices are obtained, thus to improve the repeatability of measurement. Moreover, a totally new algorithm, support vector machine (SVM) combined with partial least square (PLS) regression(SVM-PLS), is utilized to establish an effective prediction model to make a high prediction accuracy. The coefficient of determination (R2), root mean square error of prediction (RMSEP), and average relative error (ARE) are 0.944, 0.90%, and 0.80%, respectively. In comparison with the result of the traditional PLS model, the SVM residual correction greatly improves the quality of the calibration curve and makes RMSEP and ARE reduced 0.17%, thus improves the prediction accuracy, which is much better than basic PLS regression. Meanwhile, the prediction error from binder mixed semi-coke slice is significantly reduced compared to that with directly painting samples on a tape. The maximum relative errors (MRE) are 2.71% and 5.19%, and the average RSD of the characteristic peaks are 12.1% and 16.2%, respectively, indicating that the easy way with painting sample on tape has little prediction uncertainties. Finally, in a three-day random test, the average RMSEP is 1.89% and average ARE is 1.74%, which also proves the binder additive can effectively reduce the matrix effect and enhance the stability of the spectrum for semi-coke measurement. The result proposes the proper LIBS analysis on semi-coke is a feasible and promising approach for on-line prediction of such kind of coal sample.
关键词： LIBS,prediction accuracy,Laser-Induced Breakdown Spectroscopy,semi-coke,carbon content,SVM-PLS
更新于2025-09-23 15:19:57
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Concentric multipass cell enhanced double-pulse laser-induced breakdown spectroscopy for sensitive elemental analysis
摘要： Although double-pulse laser-induced breakdown spectroscopy (DP-LIBS) is regarded as a promising technique in trace element analysis, its limit of detection (LOD) is not sufficient for some applications. The enhancement of spectral signal is the key to further improve the sensitivity of DP-LIBS. To further increase the sensitivity of DP-LIBS, a concentric multipass cell (CMC) enhanced DP-LIBS (CMC-DP-LIBS) technique is proposed for the first time, which makes full use of the energy of reheating laser by multi-reflection in CMC to enhance the spectral signal and lower LOD. 2.3 times signal enhancement of Mn I 403.08 nm line and 2.3 times decrease of LOD of Mn on the surface of zinc bulk compared with traditional orthogonal reheating DP-LIBS were attained. The signal enhancement factor can reach to 3.6 theoretically with the increase of reflectivity and the sizes of mirrors of CMC. This CMC-DP-LIBS provides a new approach to further improve the sensitivity of DP-LIBS and promotes its application in trace element detection.
关键词： Double-pulse,Concentric multipass cell enhancement,Laser-induced breakdown spectroscopy,Detection limit
更新于2025-09-23 15:19:57
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Plasma chemistry produced during laser ablation of graphite in air, argon, helium and nitrogen
摘要： Laser-induced plasma chemistry produced during the ablation of graphite targets at atmospheric pressure in air, argon, helium and nitrogen was studied through time-resolved atomic and molecular emission spectroscopy. The plasma plume and plasma chemistry were generated by focusing a 6-mm diameter, 212 mJ, 1064-nm nanosecond Nd:YAG laser to a spot size of about 1 mm diameter over graphite samples of 99.9% pureness. The atomic emissions C I 247.86 nm, N I 821.50 nm and O I 777.19 nm, and the molecular bands C2 (473.71 nm) and CN (359.04 nm and 388.30 nm) were monitored as a function of time (0.2 to 220 μs). While the C I and C2 emissions followed a near-exponential decay, the CN emission in air and nitrogen showed an emission behavior characterized by two local maxima at 0.2 μs and 20-30 μs after the plasma ignition. The first maximum was explained by the early plasma chemistry produced by the ablated carbon species and the confining background gas, whereas the second maximum was attributed to atomic recombination and shock wave-induced excitation of the plasma plume. Two main effects were observed when the ablation was produced in different background gases. First, the presence of oxygen (≈21%) in air had a negligible effect on atomic lines; however, the CN emission intensity and lifetime were significantly reduced in comparison with an atmosphere of 100% nitrogen. This was attributed to the reduction of nitrogen species as reaction partners during the plasma chemistry in air. Secondly, due to the assumed higher plasma temperature in Ar, this gas favored the emission intensity and lifetime of atomic species but hindered the formation of C2 species. Because the collection optics of the emission spectroscopy system was configured in backscatter mode, which integrates over the entire plasma volume and gate time without spatial resolution, the time-resolved behavior of the plasma emissions were only related to the number density of emitters but not to specific locations in the plasma volume.
关键词： Atomic-molecular emissions,Laser-induced breakdown spectroscopy,Plasma chemistry,Graphite
更新于2025-09-23 15:19:57