Formic and acetic acids are the most abundant gaseous organic acids and play the key role in the atmospheric chemistry.In iodine-adduct chemical ionizationmass spectrometry(CIMS),the low utilization efficiency of meth...Formic and acetic acids are the most abundant gaseous organic acids and play the key role in the atmospheric chemistry.In iodine-adduct chemical ionizationmass spectrometry(CIMS),the low utilization efficiency of methyl iodide and humidity interference are two major issues of the vacuum ultraviolet(VUV)lamp initiated CIMS for on-line gaseous formic and acetic acids analysis.In this work,we present a new CIMS based on VUV lamp,and the ion-molecular reactor is separated into photoionization and chemical ionization zones by a reducer electrode.Acetone was added to the photoionization zone,and the VUV photoionization acetone provided low-energy electrons for methyl iodide to generate I−,and the addition of acetone reduced the amount of methyl iodide by 2/3.In the chemical ionization zone,a headspace vial containing ultrapure water was added for humidity calibration,and the vial changes the sensitivity as a function of humidity from ambiguity to well linear correlation(R2>0.95).With humidity calibration,the CIMS can quantitatively measure formic and acetic acids in the humidity range of 0%-88%RH.In this mode,limits of detection of 10 and 50 pptv are obtained for formic and acetic acids,respectively.And the relative standard deviation(RSD)of quantitation stability for 6 days were less than 10.5%.This CIMS was successfully used to determine the formic and acetic acids in the underground parking and ambient environment of the Shandong University campus(Qingdao,China).In addition,we developed a simple model based formic acid concentration to assess vehicular emissions.展开更多
We propose an approach for recognizing the pose and surface material of diverse objects,leveraging diffuse reflection principles and data fusion.Through theoretical analysis and the derivation of factors influencing d...We propose an approach for recognizing the pose and surface material of diverse objects,leveraging diffuse reflection principles and data fusion.Through theoretical analysis and the derivation of factors influencing diffuse reflection on objects,the method concentrates on and exploits surface information.To validate the feasibility of our theoretical research,the depth and active infrared intensity data obtained from a single time-of-flight camera are initially combined.Subsequently,these data undergo processing using feature extraction and lightweight machine-learning techniques.In addition,an optimization method is introduced to enhance the fitting of intensity.The experimental results not only visually showcase the effectiveness of our proposed method in accurately detecting the positions and surface materials of targets with varying sizes and spatial locations but also reveal that the vast majority of the sample data can achieve a recognition accuracy of 94.8%or higher.展开更多
A liquid-microjet(LJ)linear time-of-flight(TOF)mass spectrometer,coupled with a femtosecond laser ionization source,has been designed for direct measurements of mass spectra of liquid aqueous solutions.Two main featur...A liquid-microjet(LJ)linear time-of-flight(TOF)mass spectrometer,coupled with a femtosecond laser ionization source,has been designed for direct measurements of mass spectra of liquid aqueous solutions.Two main features of our designed spectrometer involve the coupling of a liquid microjet nozzle to a conventional ion optics and the application of femtosecond pulses for mass spectral ionization.The detailed design,construction,and simulation of this new spectrometer are presented.More importantly,we combined the experimental tests with the simulated electric fields and ion trajectories to investigate the performance of the designed spectrometer,especially the kind of disturbances of the nozzle electric field on the conventional ion optics.In our current design,the optimal E/R(E:extractor,R:repeller)electrode voltage ratio was found to be∼0.71 when the voltages on the R,E and G(ground)electrodes were set to be 1500,1060 and 0 V,respectively,whilst the voltage on the N nozzle electrode was required to be around 1250 V.The capability of the designed spectrometer has been demonstrated by recording the simulated mass spectra of the water,benzene and cytidine with their mass/charge ratios of 18,76 and 243,respectively.This work shall be helpful for the development of new all-liquid-phase mass spectral technology to be employed in the diagnosis of diseases by the mass analysis of human body fluids.展开更多
An experiment facility has been set up for the study of metal cluster compounds in our laboratory, which consists of a nano-electrospray ionization source, an ion transmission and focus system, and a reflectron time-o...An experiment facility has been set up for the study of metal cluster compounds in our laboratory, which consists of a nano-electrospray ionization source, an ion transmission and focus system, and a reflectron time-of-fight mass spectrometer. Taking advantage of the nano-electrospray ionization source, polyvalent ions are usually produced in the ＂ionization＂ process and the obtained mass resolution of the equipment is over 8000. The molecular ion peaks of metal cluster compounds [Au20（PPhpy2）10Cl2]（SbF6）4, where PPhpy2=bis（2- pyridyl）phenylphosphine, and [AuaAg2（C）L6]（BF4）4, where L=2-（diphenylphosphino）-5- methylpyridine, are distinguished in the respective mass spectrum, accompanied by some fragment ion peaks. In addition, the mass-to-charge ratios of the parent ions are determi- nated. Preliminary results suggest that the device is a powerful tool for the study of metal cluster compounds. It turns out that the information obtained by the instrumentation serves as an essential supplement to single crystal X-ray diffraction for structure characterization of metal cluster compounds.展开更多
Inherent complexity of plant metabolites necessitates the use of multi-dimensional information to accomplish comprehensive profiling and confirmative identification.A dimension-enhanced strategy,by offline two-dimensi...Inherent complexity of plant metabolites necessitates the use of multi-dimensional information to accomplish comprehensive profiling and confirmative identification.A dimension-enhanced strategy,by offline two-dimensional liquid chromatography/ion mobility-quadrupole time-of-flight mass spectrometry(2 D-LC/IM-QTOF-MS)enabling four-dimensional separations(2 D-LC,IM,and MS),is proposed.In combination with in-house database-driven automated peak annotation,this strategy was utilized to characterize ginsenosides simultaneously from white ginseng(WG)and red ginseng(RG).An offline 2 DLC system configuring an Xbridge Amide column and an HSS T3 column showed orthogonality 0.76 in the resolution of ginsenosides.Ginsenoside analysis was performed by data-independent high-definition MSE(HDMSE)in the negative ESI mode on a Vion?IMS-QTOF hybrid high-resolution mass spectrometer,which could better resolve ginsenosides than MSEand directly give the CCS information.An in-house ginsenoside database recording 504 known ginsenosides and 58 reference compounds,was established to assist the identification of ginsenosides.Streamlined workflows,by applying UNIFI?to automatedly annotate the HDMSEdata,were proposed.We could separate and characterize 323 ginsenosides(including 286 from WG and 306 from RG),and 125 thereof may have not been isolated from the Panax genus.The established 2 D-LC/IM-QTOF-HDMSEapproach could also act as a magnifier to probe differentiated components between WG and RG.Compared with conventional approaches,this dimensionenhanced strategy could better resolve coeluting herbal components and more efficiently,more reliably identify the multicomponents,which,we believe,offers more possibilities for the systematic exposure and confirmative identification of plant metabolites.展开更多
With the expansion of herbal medicine （HM） market, the issue on how to apply up-to- date analytical tools on qualitative analysis of HMs to assure their quality, safety and efficacy has been arousing great attention...With the expansion of herbal medicine （HM） market, the issue on how to apply up-to- date analytical tools on qualitative analysis of HMs to assure their quality, safety and efficacy has been arousing great attention. Due to its inherent characteristics of accurate mass measurements and multiple stages analysis, the integrated strategy of liquid chromatography （LC） coupled with time-of-flight mass spectrometry （TOF-MS） and ion trap mass spectrometry （IT-MS） is well-suited to be performed as qualitative analysis tool in this field. The purpose of this review is to provide an overview on the potential of this integrated strategy, including the review of general features of LC-IT-MS and LC-TOF-MS, the advantages of their combination, the common procedures for structure elucidation, the potential of LC-hybrid-IT-TOF/MS and also the summary and discussion of the applications of the integrated strategy for HM qualitative analysis （2006-2011）. The advantages and future developments of LC coupled with IT and TOF-MS are highlighted.展开更多
Detecting feature points on the human body in video frames is a key step for tracking human movements. There have been methods developed that leverage models of human pose and classification of pixels of the body imag...Detecting feature points on the human body in video frames is a key step for tracking human movements. There have been methods developed that leverage models of human pose and classification of pixels of the body image. Yet, occlusion and robustness are still open challenges. In this paper, we present an automatic, model-free feature point detection and action tracking method using a time-of-flight camera. Our method automatically detects feature points for movement abstraction. To overcome errors caused by miss-detection and occlusion, a refinement method is devised that uses the trajectory of the feature points to correct the erroneous detections. Experiments were conducted using videos acquired with a Microsoft Kinect camera and a publicly available video set and comparisons were conducted with the state-of-the-art methods. The results demonstrated that our proposed method delivered improved and reliable performance with an average accuracy in the range of 90 %.The trajectorybased refinement also demonstrated satisfactory effectiveness that recovers the detection with a success rate of 93.7 %. Our method processed a frame in an average time of 71.1 ms.展开更多
We introduce a modification of reflectron time-of-flight mass spectrometer for laser photodissociation of mass-selected ions. In our apparatus, the ions of interests were selected by a mass gate near the first space f...We introduce a modification of reflectron time-of-flight mass spectrometer for laser photodissociation of mass-selected ions. In our apparatus, the ions of interests were selected by a mass gate near the first space focus point and decelerated right after the mass gate, were then crossed by a laser beam for dissociation. The daughter ions and surviving parent ions were re-accelerated and analyzed by the reflectron time-of-flight mass spectrometer. Compared to the designs reported by other research groups, our selection-deceleration-dissociation-reacceleration approach has better daughter-parent-ions-separation, easier laser timing, and better overlapping between the ion beam and laser beam. We also conducted detailed cal- culations on the parent ion and daughter ion flight times, and provided a simplified formula for the calibration of daughter ion mass.展开更多
The double-threshold method has been widely used in ultrasonic flow measurement to determine time-of-flight(TOF)due to its low cost and ease of implementation.Performance of this method is negatively affected by the c...The double-threshold method has been widely used in ultrasonic flow measurement to determine time-of-flight(TOF)due to its low cost and ease of implementation.Performance of this method is negatively affected by the cycle-skip phenomenon which occurs frequently under inconstant working conditions,especially varied fluid temperature.This paper proposes a method to suppress the phenomenon to facilitate reliable determination of TOF in ultrasonic flow measurement.First,the double-threshold method is used to generate a feature point to segment the signal.Second,based on the correlation coefficient and signal power,judgement factors of individual signal periods are calculated to determine signal onset.Finally,a valid zero crossing which has a constant lag from the onset is selected to determine the TOF.Thus,the cycle-skip phenomenon is suppressed.Two additional modifications are proposed to eliminate the influence of varied signal frequency and low sampling rate.The proposed method was validated by an experiment based on an ultrasonic water flow sensor.Results showed that the frequently appearing cycle-skip phenomenon can be successfully suppressed by the proposed method.展开更多
BACKGROUND Neurovascular compression(NVC) is the main cause of primary trigeminal neuralgia(TN) and hemifacial spasm(HFS). Microvascular decompression(MVD) is an effective surgical method for the treatment of TN and H...BACKGROUND Neurovascular compression(NVC) is the main cause of primary trigeminal neuralgia(TN) and hemifacial spasm(HFS). Microvascular decompression(MVD) is an effective surgical method for the treatment of TN and HFS caused by NVC. The judgement of NVC is a critical step in the preoperative evaluation of MVD, which is related to the effect of MVD treatment. Magnetic resonance imaging(MRI) technology has been used to detect NVC prior to MVD for several years. Among many MRI sequences, three-dimensional time-of-flight magnetic resonance angiography(3D TOF MRA) is the most widely used. However, 3D TOF MRA has some shortcomings in detecting NVC. Therefore, 3D TOF MRA combined with high resolution T2-weighted imaging(HR T2WI) is considered to be a more effective method to detect NVC.AIM To determine the value of 3D TOF MRA combined with HR T2WI in the judgment of NVC, and thus to assess its value in the preoperative evaluation of MVD.METHODS Related studies published from inception to September 2022 based on PubMed, Embase, Web of Science, and the Cochrane Library were retrieved. Studies that investigated 3D TOF MRA combined with HR T2WI to judge NVC in patients with TN or HFS were included according to the inclusion criteria. Studies without complete data or not relevant to the research topics were excluded. The Quality Assessment of Diagnostic Accuracy Studies checklist was used to assess the quality of included studies. The publication bias of the included literature was examined by Deeks’ test. An exact binomial rendition of the bivariate mixed-effects regression model was used to synthesize data. Data analysis was performed using the MIDAS module of statistical software Stata 16.0. Two independent investigators extracted patient and study characteristics, and discrepancies were resolved by consensus. Individual and pooled sensitivities and specificities were calculated. The I_(2) statistic and Q test were used to test heterogeneity. The study was registered on the website of PROSERO(registration No. CRD42022357158).RESULTS Our search identified 595 articles, of which 12(including 855 patients) fulfilled the inclusion criteria. Bivariate analysis showed that the pooled sensitivity and specificity of 3D TOF MRA combined with HR T2WI for detecting NVC were 0.96 [95% confidence interval(CI): 0.92-0.98] and 0.92(95%CI: 0.74-0.98), respectively. The pooled positive likelihood ratio was 12.4(95%CI: 3.2-47.8), pooled negative likelihood ratio was 0.04(95%CI: 0.02-0.09), and pooled diagnostic odds ratio was 283(95%CI: 50-1620). The area under the receiver operating characteristic curve was 0.98(95%CI: 0.97-0.99). The studies showed no substantial heterogeneity(I2 = 0, Q = 0.001 P = 0.50).CONCLUSION Our results suggest that 3D TOF MRA combined with HR T2WI has excellent sensitivity and specificity for judging NVC in patients with TN or HFS. This method can be used as an effective tool for preoperative evaluation of MVD.展开更多
To predict the soft error rate for applications, it is essential to study the energy dependence of the single-event-upset(SEU) cross-section. In this work, we present a direct measurement of the SEU cross-section with...To predict the soft error rate for applications, it is essential to study the energy dependence of the single-event-upset(SEU) cross-section. In this work, we present a direct measurement of the SEU cross-section with the Back-n white neutron source at the China Spallation Neutron Source. The measured cross section is consistent with the soft error data from the manufacturer and the result suggests that the threshold energy of the SEU is about 0.5 Me V, which confirms the statement in Iwashita’s report that the threshold energy for neutron soft error is much below that of the(n, α) cross-section of silicon.In addition, an index of the effective neutron energy is suggested to characterize the similarity between a spallation neutron beam and the standard atmospheric neutron environment.展开更多
The complex composition of herbal metabolites necessitates the development of powerful analytical techniques aimed to identify the bioactive components.The seeds of Descurainia sophia(SDS)are utilized in China as a co...The complex composition of herbal metabolites necessitates the development of powerful analytical techniques aimed to identify the bioactive components.The seeds of Descurainia sophia(SDS)are utilized in China as a cough and asthma relieving agent.Herein,a dimension-enhanced integral approach,by combining ultra-high performance liquid chromatography/ion mobility-quadrupole time-of-flight mass spectrometry(UHPLC/IMQTOF-MS)and intelligent peak annotation,was developed to rapidly characterize the multicomponents from SDS.Good chromatographic separation was achieved within 38 min on a UPLC CSH C18(2.1×100 mm,1.7μm)column which was eluted by 0.1%formic acid in water(water phase)and acetonitrile(organic phase).Collision-induced dissociation-MS^(2)data were acquired by the data-independent high-definition MS^(E)(HDMS^(E))in both the negative and positive electrospray ionization modes.A major components knockout strategy was applied to improve the characterization of those minor ingredients by enhancing the injection volume.Moreover,a self-built chemistry library was established,which could be matched by the UNIFI software enabling automatic peak annotation of the obtained HDMS^(E)data.As a result of applying the intelligent peak annotation workflows and further confirmation process,a total of 53 compounds were identified or tentatively characterized from the SDS,including 29 flavonoids,one uridine derivative,four glucosides,one lignin,one phenolic compound,and 17 others.Notably,four-dimensional information related to the structure(e.g.,retention time,collision cross section,MS^(1)and MS^(2)data)was obtained for each component by the developed integral approach,and the results would greatly benefit the quality control of SDS.展开更多
It is difficult to rapidly and on-line detect trace volatile organic compounds for miniature massspectrometry due to its limited sampling volume at slow pumping speed. In this paper, we developed anew radiofrequency f...It is difficult to rapidly and on-line detect trace volatile organic compounds for miniature massspectrometry due to its limited sampling volume at slow pumping speed. In this paper, we developed anew radiofrequency field enhanced chemical ionization source （RF-ECI） with vacuum ultraviolet （VUV）lamp by coupling radiofrequency electric field and direct-current field together. The experiment resultsshowed that the sensitivity of benzene, toluene, hydrogen sulfide and other compounds increased by 2-3orders of magnitude under the introduction of RF-ECI comparing to traditional single photon ionization（SPI）. At the same time, the reagent ion of O2＋ realized the charge transfer reaction chemical ionization,and the RF-ECI effectively expanded the detection range of the VUV lamp based SPI. The VUV lamp hasinherent advantages in the on-site analytical instrument for its small size and low power consumption,and the VUV lamp based RF-ECI miniature time-of-flight mass spectrometer （TOFMS） has a limit-of-detection for H2S as low as 0.0571 mg/m3, and it is expected to be used widely in the field of on-site rapidanalvsis.展开更多
Broadband ultrasound signals will produce distortion in viscoacoustic medium, which may influence the accuracy of time-of-flight (TOF) measurement. Under the condition of single-frequency acoustic source, the wave pro...Broadband ultrasound signals will produce distortion in viscoacoustic medium, which may influence the accuracy of time-of-flight (TOF) measurement. Under the condition of single-frequency acoustic source, the wave propagation process in viscoacoustic medium was analyzed and an approximate solution of the wave propagation was given. Instances of broadband ultrasound were analyzed and simulated based on the single-frequency results. A single-frequency matching pursuits (SFMP) algorithm was then introduced to solve the waveform distortion problem. Time-frequency decomposition was applied to extracting the single-frequency compositions from broadband ultrasound signals, and then these compositions were sent to the matching pursuits (MP) algorithm for calculating the TOF parameters. Compared with the broadband signals, the shapes of extracted single-frequency signals change more slightly as distance and attenuation coefficient increase. The residuals of SFMP were far less than those of MP algorithm. Experimental results show that the SFMP algorithm is able to eliminate waveform distortion of broadband ultrasound in viscoacoustic medium, which helps improve the accuracy of TOF measurement.展开更多
Tungsten(W)is an important material in tokamak walls and divertors.The W ion charge state distribution and the dynamic behavior of ions play important roles in the investigation of plasma–wall interactions using lase...Tungsten(W)is an important material in tokamak walls and divertors.The W ion charge state distribution and the dynamic behavior of ions play important roles in the investigation of plasma–wall interactions using laser-ablation-based diagnostics such as laser-induced breakdown spectroscopy and laser-induced ablation spectroscopy.In this work,we investigate the temporal and spatial evolutions of differently charged ions in a nanosecond-laser-produced W plasma in vacuum using time-of-flight mass spectroscopy.Ions with different charge states from 1 to 7(W+to W7+)are all observed.The temporal evolutions of the differently charged ions show that ions with higher charge states have higher velocities,indicating that space separation occurs between the differently charged ion groups.Spatially-resolved mass spectroscopy measurements further demonstrate the separation phenomenon.The temporal profile can be accurately fitted by a shifted Maxwell–Boltzmann distribution,and the velocities of the differently charged ions are also obtained from the fittings.It is found that the ion velocities increase continuously from the measured position of 0.75 cm to 2.25 cm away from the target surface,which indicates that the acceleration process lasts through the period of plasma expansion.The acceleration and space separation of the differently charged ions confirm that there is a dynamic plasma sheath in the laser-produced plasma,which provides essential information for the theoretical laser-ablation model with plasma formation and expansion.展开更多
The electron impact time-of-flight(TOF) mass spectra of the title compounds were studied to establish their fragmentation processes. With the high resolution of the TOF instrument, the exact mass for each fragment was...The electron impact time-of-flight(TOF) mass spectra of the title compounds were studied to establish their fragmentation processes. With the high resolution of the TOF instrument, the exact mass for each fragment was determined. These data were used to infer the molecular formulas and the elemental compositions for all the molecular ions and fragments through software interpretation. By further applying the fragmentation regularity, the majority of ions were fully assigned. The main fragmentation pathways of the title compounds include the formation of molecular ions by the loss of R 1 groups in the 4-position and the ester groups in the 5-position. The formed ion can be further fragmented by the elimination of MeOH.展开更多
In a positron emission tomography(PET)scanner,the time-of-flight(TOF)information gives us rough event position along the line-of-response(LOR).Using the TOF information for PET image reconstruction is able to reduce i...In a positron emission tomography(PET)scanner,the time-of-flight(TOF)information gives us rough event position along the line-of-response(LOR).Using the TOF information for PET image reconstruction is able to reduce image noise.The state-of-the-art TOF PET image reconstruction uses iterative algorithms.This study introduces an analytic TOF PET algorithm that focuses on three-dimensional(3D)reconstruction.The proposed algorithm is in the form of backprojection filtering,in which the backprojection is performed first by using a time-resolution profile function,and then a 3D filter is applied to the backprojected image.For the list-mode data,the backprojection is carried out in the event-by-event fashion,and the timing resolution determined weighting function is used along the projection LOR.Computer simulations are carried out to verify the feasibility of the proposed algorithm.展开更多
The time-of-flight mass spectrometry(TOF-MS),one of the mass spectrometry techniques,has been widely applied in the field of rapid screening of food hazard factors as a superior analysis technique because of its wide ...The time-of-flight mass spectrometry(TOF-MS),one of the mass spectrometry techniques,has been widely applied in the field of rapid screening of food hazard factors as a superior analysis technique because of its wide mass range,high resolution and mass measurement accuracy,high sensitivity and high analysis speed.In this paper,research progresses of TOF-MS on the detection of food additives,food contaminants and residues,illegal additives,pesticide residues,veterinary drug residues and mycotoxin were reviewed,and its probable approaching applications were prospected.展开更多
基金supported by the National Special Fund for the Development of Major Research Equipment and Instrument(No.2020YFF01014503)the Young Taishan Scholars(No.tsqn201909039)the College 20 Project fromJi Nan Science&Technology Bureau(No.2021GXRC058).
文摘Formic and acetic acids are the most abundant gaseous organic acids and play the key role in the atmospheric chemistry.In iodine-adduct chemical ionizationmass spectrometry(CIMS),the low utilization efficiency of methyl iodide and humidity interference are two major issues of the vacuum ultraviolet(VUV)lamp initiated CIMS for on-line gaseous formic and acetic acids analysis.In this work,we present a new CIMS based on VUV lamp,and the ion-molecular reactor is separated into photoionization and chemical ionization zones by a reducer electrode.Acetone was added to the photoionization zone,and the VUV photoionization acetone provided low-energy electrons for methyl iodide to generate I−,and the addition of acetone reduced the amount of methyl iodide by 2/3.In the chemical ionization zone,a headspace vial containing ultrapure water was added for humidity calibration,and the vial changes the sensitivity as a function of humidity from ambiguity to well linear correlation(R2>0.95).With humidity calibration,the CIMS can quantitatively measure formic and acetic acids in the humidity range of 0%-88%RH.In this mode,limits of detection of 10 and 50 pptv are obtained for formic and acetic acids,respectively.And the relative standard deviation(RSD)of quantitation stability for 6 days were less than 10.5%.This CIMS was successfully used to determine the formic and acetic acids in the underground parking and ambient environment of the Shandong University campus(Qingdao,China).In addition,we developed a simple model based formic acid concentration to assess vehicular emissions.
基金supported by the Shaanxi Province Innovation Talent Promotion Program-Science and Technology Innovation Team(Grant No.2023-CX-TD-03).
文摘We propose an approach for recognizing the pose and surface material of diverse objects,leveraging diffuse reflection principles and data fusion.Through theoretical analysis and the derivation of factors influencing diffuse reflection on objects,the method concentrates on and exploits surface information.To validate the feasibility of our theoretical research,the depth and active infrared intensity data obtained from a single time-of-flight camera are initially combined.Subsequently,these data undergo processing using feature extraction and lightweight machine-learning techniques.In addition,an optimization method is introduced to enhance the fitting of intensity.The experimental results not only visually showcase the effectiveness of our proposed method in accurately detecting the positions and surface materials of targets with varying sizes and spatial locations but also reveal that the vast majority of the sample data can achieve a recognition accuracy of 94.8%or higher.
基金supported by the Knowledge Innovation Program of Wuhan-Basic Research(Nos.2023020201010084,2022010801010134)the National Key Research and Development Program of China(No.2019YFA0307700)the National Natural Science Foundation of China(Nos.12274418,22273116,12074389,11974381,22363011).
文摘A liquid-microjet(LJ)linear time-of-flight(TOF)mass spectrometer,coupled with a femtosecond laser ionization source,has been designed for direct measurements of mass spectra of liquid aqueous solutions.Two main features of our designed spectrometer involve the coupling of a liquid microjet nozzle to a conventional ion optics and the application of femtosecond pulses for mass spectral ionization.The detailed design,construction,and simulation of this new spectrometer are presented.More importantly,we combined the experimental tests with the simulated electric fields and ion trajectories to investigate the performance of the designed spectrometer,especially the kind of disturbances of the nozzle electric field on the conventional ion optics.In our current design,the optimal E/R(E:extractor,R:repeller)electrode voltage ratio was found to be∼0.71 when the voltages on the R,E and G(ground)electrodes were set to be 1500,1060 and 0 V,respectively,whilst the voltage on the N nozzle electrode was required to be around 1250 V.The capability of the designed spectrometer has been demonstrated by recording the simulated mass spectra of the water,benzene and cytidine with their mass/charge ratios of 18,76 and 243,respectively.This work shall be helpful for the development of new all-liquid-phase mass spectral technology to be employed in the diagnosis of diseases by the mass analysis of human body fluids.
文摘An experiment facility has been set up for the study of metal cluster compounds in our laboratory, which consists of a nano-electrospray ionization source, an ion transmission and focus system, and a reflectron time-of-fight mass spectrometer. Taking advantage of the nano-electrospray ionization source, polyvalent ions are usually produced in the ＂ionization＂ process and the obtained mass resolution of the equipment is over 8000. The molecular ion peaks of metal cluster compounds [Au20（PPhpy2）10Cl2]（SbF6）4, where PPhpy2=bis（2- pyridyl）phenylphosphine, and [AuaAg2（C）L6]（BF4）4, where L=2-（diphenylphosphino）-5- methylpyridine, are distinguished in the respective mass spectrum, accompanied by some fragment ion peaks. In addition, the mass-to-charge ratios of the parent ions are determi- nated. Preliminary results suggest that the device is a powerful tool for the study of metal cluster compounds. It turns out that the information obtained by the instrumentation serves as an essential supplement to single crystal X-ray diffraction for structure characterization of metal cluster compounds.
基金the National Natural Science Foundation of China(Grant No.81872996)the State Key Research and Development Project(Grant No.2017YFC1702104)+1 种基金the State Key Project for the Creation of Major New Drugs(2018ZX09711001-009-010)the Tianjin Municipal Education Commission Research Project(Grant No.2017ZD07)。
文摘Inherent complexity of plant metabolites necessitates the use of multi-dimensional information to accomplish comprehensive profiling and confirmative identification.A dimension-enhanced strategy,by offline two-dimensional liquid chromatography/ion mobility-quadrupole time-of-flight mass spectrometry(2 D-LC/IM-QTOF-MS)enabling four-dimensional separations(2 D-LC,IM,and MS),is proposed.In combination with in-house database-driven automated peak annotation,this strategy was utilized to characterize ginsenosides simultaneously from white ginseng(WG)and red ginseng(RG).An offline 2 DLC system configuring an Xbridge Amide column and an HSS T3 column showed orthogonality 0.76 in the resolution of ginsenosides.Ginsenoside analysis was performed by data-independent high-definition MSE(HDMSE)in the negative ESI mode on a Vion?IMS-QTOF hybrid high-resolution mass spectrometer,which could better resolve ginsenosides than MSEand directly give the CCS information.An in-house ginsenoside database recording 504 known ginsenosides and 58 reference compounds,was established to assist the identification of ginsenosides.Streamlined workflows,by applying UNIFI?to automatedly annotate the HDMSEdata,were proposed.We could separate and characterize 323 ginsenosides(including 286 from WG and 306 from RG),and 125 thereof may have not been isolated from the Panax genus.The established 2 D-LC/IM-QTOF-HDMSEapproach could also act as a magnifier to probe differentiated components between WG and RG.Compared with conventional approaches,this dimensionenhanced strategy could better resolve coeluting herbal components and more efficiently,more reliably identify the multicomponents,which,we believe,offers more possibilities for the systematic exposure and confirmative identification of plant metabolites.
文摘With the expansion of herbal medicine （HM） market, the issue on how to apply up-to- date analytical tools on qualitative analysis of HMs to assure their quality, safety and efficacy has been arousing great attention. Due to its inherent characteristics of accurate mass measurements and multiple stages analysis, the integrated strategy of liquid chromatography （LC） coupled with time-of-flight mass spectrometry （TOF-MS） and ion trap mass spectrometry （IT-MS） is well-suited to be performed as qualitative analysis tool in this field. The purpose of this review is to provide an overview on the potential of this integrated strategy, including the review of general features of LC-IT-MS and LC-TOF-MS, the advantages of their combination, the common procedures for structure elucidation, the potential of LC-hybrid-IT-TOF/MS and also the summary and discussion of the applications of the integrated strategy for HM qualitative analysis （2006-2011）. The advantages and future developments of LC coupled with IT and TOF-MS are highlighted.
文摘Detecting feature points on the human body in video frames is a key step for tracking human movements. There have been methods developed that leverage models of human pose and classification of pixels of the body image. Yet, occlusion and robustness are still open challenges. In this paper, we present an automatic, model-free feature point detection and action tracking method using a time-of-flight camera. Our method automatically detects feature points for movement abstraction. To overcome errors caused by miss-detection and occlusion, a refinement method is devised that uses the trajectory of the feature points to correct the erroneous detections. Experiments were conducted using videos acquired with a Microsoft Kinect camera and a publicly available video set and comparisons were conducted with the state-of-the-art methods. The results demonstrated that our proposed method delivered improved and reliable performance with an average accuracy in the range of 90 %.The trajectorybased refinement also demonstrated satisfactory effectiveness that recovers the detection with a success rate of 93.7 %. Our method processed a frame in an average time of 71.1 ms.
基金V. ACKNOWLEDGMENTS This work supported by the National Natural Science Foundation of China （No.20853001）. We thank Professor Qi-he Zhu and Professor Zhen Gao for valuable discussions.
文摘We introduce a modification of reflectron time-of-flight mass spectrometer for laser photodissociation of mass-selected ions. In our apparatus, the ions of interests were selected by a mass gate near the first space focus point and decelerated right after the mass gate, were then crossed by a laser beam for dissociation. The daughter ions and surviving parent ions were re-accelerated and analyzed by the reflectron time-of-flight mass spectrometer. Compared to the designs reported by other research groups, our selection-deceleration-dissociation-reacceleration approach has better daughter-parent-ions-separation, easier laser timing, and better overlapping between the ion beam and laser beam. We also conducted detailed cal- culations on the parent ion and daughter ion flight times, and provided a simplified formula for the calibration of daughter ion mass.
基金Project supported by the Science Fund for Creative Research Groups of National Natural Science Foundation of China(No.51821093)。
文摘The double-threshold method has been widely used in ultrasonic flow measurement to determine time-of-flight(TOF)due to its low cost and ease of implementation.Performance of this method is negatively affected by the cycle-skip phenomenon which occurs frequently under inconstant working conditions,especially varied fluid temperature.This paper proposes a method to suppress the phenomenon to facilitate reliable determination of TOF in ultrasonic flow measurement.First,the double-threshold method is used to generate a feature point to segment the signal.Second,based on the correlation coefficient and signal power,judgement factors of individual signal periods are calculated to determine signal onset.Finally,a valid zero crossing which has a constant lag from the onset is selected to determine the TOF.Thus,the cycle-skip phenomenon is suppressed.Two additional modifications are proposed to eliminate the influence of varied signal frequency and low sampling rate.The proposed method was validated by an experiment based on an ultrasonic water flow sensor.Results showed that the frequently appearing cycle-skip phenomenon can be successfully suppressed by the proposed method.
基金Supported by the Key Research and Development Plan of Shaanxi Province,No.2021SF-298.
文摘BACKGROUND Neurovascular compression(NVC) is the main cause of primary trigeminal neuralgia(TN) and hemifacial spasm(HFS). Microvascular decompression(MVD) is an effective surgical method for the treatment of TN and HFS caused by NVC. The judgement of NVC is a critical step in the preoperative evaluation of MVD, which is related to the effect of MVD treatment. Magnetic resonance imaging(MRI) technology has been used to detect NVC prior to MVD for several years. Among many MRI sequences, three-dimensional time-of-flight magnetic resonance angiography(3D TOF MRA) is the most widely used. However, 3D TOF MRA has some shortcomings in detecting NVC. Therefore, 3D TOF MRA combined with high resolution T2-weighted imaging(HR T2WI) is considered to be a more effective method to detect NVC.AIM To determine the value of 3D TOF MRA combined with HR T2WI in the judgment of NVC, and thus to assess its value in the preoperative evaluation of MVD.METHODS Related studies published from inception to September 2022 based on PubMed, Embase, Web of Science, and the Cochrane Library were retrieved. Studies that investigated 3D TOF MRA combined with HR T2WI to judge NVC in patients with TN or HFS were included according to the inclusion criteria. Studies without complete data or not relevant to the research topics were excluded. The Quality Assessment of Diagnostic Accuracy Studies checklist was used to assess the quality of included studies. The publication bias of the included literature was examined by Deeks’ test. An exact binomial rendition of the bivariate mixed-effects regression model was used to synthesize data. Data analysis was performed using the MIDAS module of statistical software Stata 16.0. Two independent investigators extracted patient and study characteristics, and discrepancies were resolved by consensus. Individual and pooled sensitivities and specificities were calculated. The I_(2) statistic and Q test were used to test heterogeneity. The study was registered on the website of PROSERO(registration No. CRD42022357158).RESULTS Our search identified 595 articles, of which 12(including 855 patients) fulfilled the inclusion criteria. Bivariate analysis showed that the pooled sensitivity and specificity of 3D TOF MRA combined with HR T2WI for detecting NVC were 0.96 [95% confidence interval(CI): 0.92-0.98] and 0.92(95%CI: 0.74-0.98), respectively. The pooled positive likelihood ratio was 12.4(95%CI: 3.2-47.8), pooled negative likelihood ratio was 0.04(95%CI: 0.02-0.09), and pooled diagnostic odds ratio was 283(95%CI: 50-1620). The area under the receiver operating characteristic curve was 0.98(95%CI: 0.97-0.99). The studies showed no substantial heterogeneity(I2 = 0, Q = 0.001 P = 0.50).CONCLUSION Our results suggest that 3D TOF MRA combined with HR T2WI has excellent sensitivity and specificity for judging NVC in patients with TN or HFS. This method can be used as an effective tool for preoperative evaluation of MVD.
基金supported by the National Natural Science Foundation of China (Grant Nos. 2032165 and 62004158)the National Key Scientific Instrument and Equipment Development Project of China (Grant No. 52127817)+1 种基金the State Key Laboratory of Particle Detection and Electronics (Grant Nos. SKLPDE-ZZ-201801 and SKLPDE-ZZ-202008)the Special Funds for Science and Technology Innovation Strategy of Guangdong Province, China (Grant No. 2018A0303130030)。
文摘To predict the soft error rate for applications, it is essential to study the energy dependence of the single-event-upset(SEU) cross-section. In this work, we present a direct measurement of the SEU cross-section with the Back-n white neutron source at the China Spallation Neutron Source. The measured cross section is consistent with the soft error data from the manufacturer and the result suggests that the threshold energy of the SEU is about 0.5 Me V, which confirms the statement in Iwashita’s report that the threshold energy for neutron soft error is much below that of the(n, α) cross-section of silicon.In addition, an index of the effective neutron energy is suggested to characterize the similarity between a spallation neutron beam and the standard atmospheric neutron environment.
基金This work was financially supported by the National Key Research and Development Program of China(Grant No.2018YFC1704500)Tianjin Committee of Science and Technology of China(Grant No.21ZYJDJC00080)National Natural Science Foundation of China(Grant No.81872996).
文摘The complex composition of herbal metabolites necessitates the development of powerful analytical techniques aimed to identify the bioactive components.The seeds of Descurainia sophia(SDS)are utilized in China as a cough and asthma relieving agent.Herein,a dimension-enhanced integral approach,by combining ultra-high performance liquid chromatography/ion mobility-quadrupole time-of-flight mass spectrometry(UHPLC/IMQTOF-MS)and intelligent peak annotation,was developed to rapidly characterize the multicomponents from SDS.Good chromatographic separation was achieved within 38 min on a UPLC CSH C18(2.1×100 mm,1.7μm)column which was eluted by 0.1%formic acid in water(water phase)and acetonitrile(organic phase).Collision-induced dissociation-MS^(2)data were acquired by the data-independent high-definition MS^(E)(HDMS^(E))in both the negative and positive electrospray ionization modes.A major components knockout strategy was applied to improve the characterization of those minor ingredients by enhancing the injection volume.Moreover,a self-built chemistry library was established,which could be matched by the UNIFI software enabling automatic peak annotation of the obtained HDMS^(E)data.As a result of applying the intelligent peak annotation workflows and further confirmation process,a total of 53 compounds were identified or tentatively characterized from the SDS,including 29 flavonoids,one uridine derivative,four glucosides,one lignin,one phenolic compound,and 17 others.Notably,four-dimensional information related to the structure(e.g.,retention time,collision cross section,MS^(1)and MS^(2)data)was obtained for each component by the developed integral approach,and the results would greatly benefit the quality control of SDS.
基金financially supported by the National Natural Science Foundation of China(Nos.21375129 and 21675155)
文摘It is difficult to rapidly and on-line detect trace volatile organic compounds for miniature massspectrometry due to its limited sampling volume at slow pumping speed. In this paper, we developed anew radiofrequency field enhanced chemical ionization source （RF-ECI） with vacuum ultraviolet （VUV）lamp by coupling radiofrequency electric field and direct-current field together. The experiment resultsshowed that the sensitivity of benzene, toluene, hydrogen sulfide and other compounds increased by 2-3orders of magnitude under the introduction of RF-ECI comparing to traditional single photon ionization（SPI）. At the same time, the reagent ion of O2＋ realized the charge transfer reaction chemical ionization,and the RF-ECI effectively expanded the detection range of the VUV lamp based SPI. The VUV lamp hasinherent advantages in the on-site analytical instrument for its small size and low power consumption,and the VUV lamp based RF-ECI miniature time-of-flight mass spectrometer （TOFMS） has a limit-of-detection for H2S as low as 0.0571 mg/m3, and it is expected to be used widely in the field of on-site rapidanalvsis.
基金Supported by National Natural Science Foundation of China (No.30800240 and No.60901043)
文摘Broadband ultrasound signals will produce distortion in viscoacoustic medium, which may influence the accuracy of time-of-flight (TOF) measurement. Under the condition of single-frequency acoustic source, the wave propagation process in viscoacoustic medium was analyzed and an approximate solution of the wave propagation was given. Instances of broadband ultrasound were analyzed and simulated based on the single-frequency results. A single-frequency matching pursuits (SFMP) algorithm was then introduced to solve the waveform distortion problem. Time-frequency decomposition was applied to extracting the single-frequency compositions from broadband ultrasound signals, and then these compositions were sent to the matching pursuits (MP) algorithm for calculating the TOF parameters. Compared with the broadband signals, the shapes of extracted single-frequency signals change more slightly as distance and attenuation coefficient increase. The residuals of SFMP were far less than those of MP algorithm. Experimental results show that the SFMP algorithm is able to eliminate waveform distortion of broadband ultrasound in viscoacoustic medium, which helps improve the accuracy of TOF measurement.
基金supported by the National Key R&D Program of China(No.2017YFE0301304)National Natural Science Foundation of China(No.12005034)the China Postdoctoral Science Foundation(No.2019M661087)supported by the US Department of Energy,Office of Defense Nuclear Nonproliferation Research and Development,under contract number DE-AC02-05CH11231 at the Lawrence Berkeley National Laboratory。
文摘Tungsten(W)is an important material in tokamak walls and divertors.The W ion charge state distribution and the dynamic behavior of ions play important roles in the investigation of plasma–wall interactions using laser-ablation-based diagnostics such as laser-induced breakdown spectroscopy and laser-induced ablation spectroscopy.In this work,we investigate the temporal and spatial evolutions of differently charged ions in a nanosecond-laser-produced W plasma in vacuum using time-of-flight mass spectroscopy.Ions with different charge states from 1 to 7(W+to W7+)are all observed.The temporal evolutions of the differently charged ions show that ions with higher charge states have higher velocities,indicating that space separation occurs between the differently charged ion groups.Spatially-resolved mass spectroscopy measurements further demonstrate the separation phenomenon.The temporal profile can be accurately fitted by a shifted Maxwell–Boltzmann distribution,and the velocities of the differently charged ions are also obtained from the fittings.It is found that the ion velocities increase continuously from the measured position of 0.75 cm to 2.25 cm away from the target surface,which indicates that the acceleration process lasts through the period of plasma expansion.The acceleration and space separation of the differently charged ions confirm that there is a dynamic plasma sheath in the laser-produced plasma,which provides essential information for the theoretical laser-ablation model with plasma formation and expansion.
基金National Natural Science Foundation of China(No.2 0 332 0 2 0 )
文摘The electron impact time-of-flight(TOF) mass spectra of the title compounds were studied to establish their fragmentation processes. With the high resolution of the TOF instrument, the exact mass for each fragment was determined. These data were used to infer the molecular formulas and the elemental compositions for all the molecular ions and fragments through software interpretation. By further applying the fragmentation regularity, the majority of ions were fully assigned. The main fragmentation pathways of the title compounds include the formation of molecular ions by the loss of R 1 groups in the 4-position and the ester groups in the 5-position. The formed ion can be further fragmented by the elimination of MeOH.
文摘In a positron emission tomography(PET)scanner,the time-of-flight(TOF)information gives us rough event position along the line-of-response(LOR).Using the TOF information for PET image reconstruction is able to reduce image noise.The state-of-the-art TOF PET image reconstruction uses iterative algorithms.This study introduces an analytic TOF PET algorithm that focuses on three-dimensional(3D)reconstruction.The proposed algorithm is in the form of backprojection filtering,in which the backprojection is performed first by using a time-resolution profile function,and then a 3D filter is applied to the backprojected image.For the list-mode data,the backprojection is carried out in the event-by-event fashion,and the timing resolution determined weighting function is used along the projection LOR.Computer simulations are carried out to verify the feasibility of the proposed algorithm.
基金Supported by Phase II Modern Agricultural Industry Technology System Innovation Team Construction Project of Hebei Province(HBCT2018120207)Key R&D Projects of Hebei Province(19227516D)Tangshan Institute of Industrial Technology for Functional Agricultural Products(2019TY003b)。
文摘The time-of-flight mass spectrometry(TOF-MS),one of the mass spectrometry techniques,has been widely applied in the field of rapid screening of food hazard factors as a superior analysis technique because of its wide mass range,high resolution and mass measurement accuracy,high sensitivity and high analysis speed.In this paper,research progresses of TOF-MS on the detection of food additives,food contaminants and residues,illegal additives,pesticide residues,veterinary drug residues and mycotoxin were reviewed,and its probable approaching applications were prospected.
