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
Strong feld-induced nonsequential double ionization(NSDI)is a signifcant multi-electron phenomenon that provides crucial insights into understanding electron correlation and multiple ionization of atoms and molecules,...Strong feld-induced nonsequential double ionization(NSDI)is a signifcant multi-electron phenomenon that provides crucial insights into understanding electron correlation and multiple ionization of atoms and molecules,but it is typically unattainable in a circularly polarized laser pulse,especially for long-wavelength lasers.We present evidence that NSDI can occur in the presence of a near-infrared or beyond laser pulse by introducing a bowtie-nanotip.The laser-induced local plasmon can alter the local ellipticity of the feld,thereby enabling NSDI through elliptical trajectories that facilitate recollisions with parent atoms.An oval-shaped momentum distribution of recoiled ions provides evidence for the modifcation of trajectories by the aligned nanotips.Our study introduces an innovative control knob to manipulate NSDI and electron dynamics through the utilization of nanostructures.展开更多
Traditional electrospray ionization tandem mass spectrometry(ESI-MS^(n))has been a powerful tool in diverse research areas,however,it faces great limitations in the study of protein-small molecule interactions.In this...Traditional electrospray ionization tandem mass spectrometry(ESI-MS^(n))has been a powerful tool in diverse research areas,however,it faces great limitations in the study of protein-small molecule interactions.In this article,the state-of-the-art temperature-controlled electrospray ionization tandem mass spectrometry(TC-ESI-MS^(n))is applied to investigate interactions between ubiquitin and two flavonol molecules,respectively.The combination of collision-induced dissociation(CID)and MS solution-melting experiments facilitates the understanding of flavonol-protein interactions in a new dimension across varying temperature ranges.While structural changes of proteins disturbed by small molecules are unseen in ESI-MS^(n),TC-ESI-MS^(n)allows a simultaneous assessment of the stability of the complex in both gas and liquid phases under various temperature conditions,meanwhile investigating the impact on the protein’s structure and tracking changes in thermodynamic data,and the characteristics of structural intermediates.展开更多
Accurate determination of lung cancer margins at the molecular level is of great significance to determine the optimal extent of resection during surgical operation and reduce the risk of postoperative recurrence.In t...Accurate determination of lung cancer margins at the molecular level is of great significance to determine the optimal extent of resection during surgical operation and reduce the risk of postoperative recurrence.In this study,internal extractive electrospray ionization mass spectrometry(i EESI-MS)was used to trace potential molecular tumor margins in lung cancer tissue.Molecular differential model for the determination of lung cancer tumor margin was established via partial least-squares discriminant analysis(PLS-DA)of iEESI-MS data collected from lung tissue pieces within cancer tumor area and iEESI-MS data collected from lung tissue pieces outside cancer tumor area.Proof-of-concept data demonstrate that the developed molecular differential model yields ca.1-2 mm wider potential molecular tumor margin of a lung cancer compared to the conventional histological analysis,showing promising potential of iEESI-MS to increase the accuracy of tumor margins determination and lower risk of lung cancer postoperative recurrence.Furthermore,our results revealed that creatine and taurine showed positive correlations with lung cancer.展开更多
In this study, we provide a detailed case study of the X-pattern of equatorial ionization anomaly(EIA) observed on the night of September 12, 2021 by the Global-scale Observations of the Limb and Disk(GOLD) mission. U...In this study, we provide a detailed case study of the X-pattern of equatorial ionization anomaly(EIA) observed on the night of September 12, 2021 by the Global-scale Observations of the Limb and Disk(GOLD) mission. Unlike most previous studies about the X-pattern observed under the severely disturbed background ionosphere, this event is observed under geomagnetically quiet and low solar activity conditions. GOLD's continuous observations reveal that the X-pattern intensity evolves with local time, while its center's longitude remains constant. The total electron content(TEC) data derived from the ground-based Global Navigation Satellite System(GNSS) network aligns well with GOLD observations in capturing the formation of the X-pattern, extending coverage to areas beyond GOLD's observational reach. Additionally, the ESA's Swarm mission show that both sides of the X-pattern can coincide with the occurrence of small-scale equatorial plasma bubbles(EPBs). To further analyze the possible drivers of the X-pattern, observations from the Ionospheric Connection Explorer(ICON) satellite were used. It shows that the latitudinal expansion(or width) between the EIA crests in two hemispheres is proportional(or inversely proportional) to the upward(or downward) plasma drift velocity, which suggests that the zonal electric field should have a notable influence on the formation of EIA X-pattern. Further simulations using the SAMI2 model support this mechanism, as the X-pattern of EIA is successfully reproduced by setting the vertical plasma drift to different values at different longitudes.展开更多
Selenium is one of the important trace elements in the human body.Its deficiency will directly affect human health.With people's attention to health,the content of selenium in food has gradually attracted attentio...Selenium is one of the important trace elements in the human body.Its deficiency will directly affect human health.With people's attention to health,the content of selenium in food has gradually attracted attention.However,detecting selenium compounds in complex samples remains a challenge.In this work,we built an online heating-reaction device.This device combines the electrospray extraction ionization mass spectrometry(EESI-MS)with the heating reaction device,which can simultaneously detect various selenium compounds in complex liquid samples.Under acidic conditions,the sample was heated and catalyzed by a heating reaction device,so that the SeO~(2-)_(3)and O-phenylenediamine(OPD)could generate 1,3-dihydro-2,1,3-benzoselenadiazole.Based on the above reactions,we can detect organic selenium,inorganic selenium and other compounds in liquid samples by organic mass spectrometry.In this experiment,we determined the content of three forms of selenium:selenomethionine(SeMet),l-selenocystine(SeCys(2)),and sodium selenite.The calibration curves for SeMet,SeCys(2),and sodium selenite showed strong linearity within a range of 0.50-50.00μg/L.The limits of detection(LOD)for the three compounds were 0.22,0.27,and 0.41μg/L,respectively.The limits of quantification(LOQ)were 0.68,0.81,and 1.23μg/L,respectively.Spiked recoveries at three levels ranged from 98.8%to 106.1%.In addition,this method can simultaneously detect three selenium compounds and three other specific chemical components in tea infusion samples,providing a rapid and efficient method for identifying tea quality.展开更多
The ultrafast excitation dynamics of atoms and molecules exposed to circularly polarized two-color(CPTC)laser fields constitute a fascinating topic in attosecond science. Although extensive research has established th...The ultrafast excitation dynamics of atoms and molecules exposed to circularly polarized two-color(CPTC)laser fields constitute a fascinating topic in attosecond science. Although extensive research has established the relationship between the Rydberg state excitation(RSE) yields and the CPTC field parameters, such as field amplitude ratios and helicity of two components, the role of the relative phase(φ) in modulating RSE efficiency remains unclear. In this work, we theoretically investigate the φ dependence of RSE and ionization yields in the co-rotating and counter-rotating circularly polarized two-color(CPTC) few-cycle laser fields by a semiclassical model. We find that, in co-rotating CPTC fields, both RSE and ionization yields display pronounced oscillations as a function of φ and these oscillations are significantly suppressed in the counter-rotating configuration, particularly for ionization yields. Moreover, the ratio of RSE to ionization yields exhibits an out-of-phase oscillatory pattern between low-and high-intensity regimes. These results can be comprehended by the unique feature of φ dependence of CPTC few-cycle fields, based on our semiclassical analysis. Our results demonstrate that phase-controlled CPTC fields offer a versatile tool for steering ultrafast ionization and RSE dynamics of atoms and molecules.展开更多
This study analytically examines the ionization of atoms in strong near-circular laser fields.The classic Keldysh-Rutherford(KR)Coulomb-scattering(CS)model[Phys.Rev.Lett.121123201(2018)]successfully explained the atto...This study analytically examines the ionization of atoms in strong near-circular laser fields.The classic Keldysh-Rutherford(KR)Coulomb-scattering(CS)model[Phys.Rev.Lett.121123201(2018)]successfully explained the attoclock experimental curve for the H atom at lower laser intensities.Here,we develop a semiclassical model that includes the initial conditions related to the quantum properties of tunneling in the KR model at the beginning of the scattering process.This model is able to explain recent attoclock experimental curves over a wider range of laser and atomic parameters.Our results show the importance of system symmetry and quantum effects in attoclock measurements,suggesting the complex role of the Coulomb potential in strong-field ionization.展开更多
We propose a method to characterize the features of a cold strontium cloud in a magneto-optical trap(MOT)through the photoionization of cold Sr atoms in a custom-designed reaction microscope.Sr atoms in the dark state...We propose a method to characterize the features of a cold strontium cloud in a magneto-optical trap(MOT)through the photoionization of cold Sr atoms in a custom-designed reaction microscope.Sr atoms in the dark state of 5s5p3P2 populated via the cascade transition 5s5p^(1)P_(1)→5s4d^(1)D_(2)→5s5p^(3)P_(2)accumulate a significant fraction,giving a long lifetime of 520 s.These atoms in the dark state are subsequently trapped by the gradient magnetic field of the MOT.By scanning the Sr+momentum distributions ionized with an 800 nm infrared femtosecond laser,we are able to outline the size of~0.55 mm in radius and the temperature of~0.40 mK for the dark-state atoms,which is significantly cooler than the MOT temperature of 3.3 mK trapped in the 461 nm.The size of MOT exhibits an oblate spheroidal distribution with a radius of approximately 0.35 mm and 0.55 mm,extracted with momenta of photoion and absorption imaging,respectively.The results using the photoion momenta are consistent with the expected results from absorption imaging,which confirms the method's reliability.The advantage of this method is the ability to simultaneously characterize the distribution information of atoms in different initial states within the cold atomic cloud.展开更多
The direct and dissociative ionizations of oxygen molecule are investigated experimen-tally by electron collision with energies from 350 eV to 8000 eV.The absolute ionization cross sections for the product ions(O_(2)^...The direct and dissociative ionizations of oxygen molecule are investigated experimen-tally by electron collision with energies from 350 eV to 8000 eV.The absolute ionization cross sections for the product ions(O_(2)^(2+),O_(2)^(2+)O^(+),O^(2+),and their total)and two Coulomb explosion channels(O^(+)+O^(+)and O^(2+)+O^(+))are obtained by putting the data of O^(2+)on the scale of Ar+from O_(2)and Ar gases mixed with a fixed relative flow ratio of 1:1.The experimental errors are assessed by taking uncertainties of various factors into account.The present absolute cross sections are well consistent with the previous data in the overlapped energy range below 1000 eV.展开更多
With a three-dimensional semiclassical ensemble method, we theoretically investigated the nonsequential double ionization of Ar driven by the spatially inhomogeneous few-cycle negatively chirped laser pulses. Our resu...With a three-dimensional semiclassical ensemble method, we theoretically investigated the nonsequential double ionization of Ar driven by the spatially inhomogeneous few-cycle negatively chirped laser pulses. Our results show that the recollision time window can be precisely controlled within an isolated time interval of several hundred attoseconds, which is useful for understanding the subcycle correlated electron dynamics. More interestingly, the correlated electron momentum distribution (CEMD) exhibits a strong dependence on laser intensity. That is, at lower laser intensity, CEMD is located in the first quadrant. As the laser intensity increases,CEMD shifts almost completely to the second and fourth quadrants, and then gradually to the third quadrant.The underlying physics governing the CEMD's dependence on laser intensity is explained.展开更多
Electronic processes within atoms and molecules reside on the timescale of attoseconds. Recent advances in the laserbased pump-probe interrogation techniques have made possible the temporal resolution of ultrafast ele...Electronic processes within atoms and molecules reside on the timescale of attoseconds. Recent advances in the laserbased pump-probe interrogation techniques have made possible the temporal resolution of ultrafast electronic processes on the attosecond timescale, including photoionization and tunneling ionization. These interrogation techniques include the attosecond streak camera, the reconstruction of attosecond beating by interference of two-photon transitions, and the attoclock. While the former two are usually employed to study photoionization processes, the latter is typically used to investigate tunneling ionization. In this review, we briefly overview these timing techniques towards an attosecond temporal resolution of ionization processes in atoms and molecules under intense laser fields. In particular, we review the backpropagation method, which is a novel hybrid quantum-classical approach towards the full characterization of tunneling ionization dynamics. Continued advances in the interrogation techniques promise to pave the pathway towards the exploration of ever faster dynamical processes on an ever shorter timescale.展开更多
Cancer cell spheroids(CCS) are a valuable three-dimensional cell model in cancer studies because they could replicate numerous characteristics of solid tumors. Increasing researches have used matrix-assisted laser des...Cancer cell spheroids(CCS) are a valuable three-dimensional cell model in cancer studies because they could replicate numerous characteristics of solid tumors. Increasing researches have used matrix-assisted laser desorption/ionization mass spectrometry imaging(MALDI-MSI) to investigate the spatial distribution of endogenous compounds(e.g., lipids) in CCS. However, only limited lipid species can be detected owing to a low ion yield by using MALDI. Besides, it is still challenging to fully characterize the structural diversity of lipids due to the existence of isomeric/isobaric species. Here, we carried out the initial application of MALDI coupled with laser-postionization(MALDI-2) and trapped ion mobility spectrometry(TIMS) imaging in HCT116 colon CCS to address these challenges. We demonstrated that MALDI-2 is capable of detecting more number and classes of lipids in HCT116 colon CCS with higher signal intensities than MALDI. TIMS could successfully separate numerous isobaric/isomeric species of lipids in CCS. Interestingly, we found that some isomeric/isobaric species have totally different spatial distributions in colon CCS. Further MS/MS imaging analysis was employed to determine the compositions of fatty acid chains for isomeric species by examining disparities in signal intensities and spatial distributions of product ions. This work stresses the robust ability of TIMS and MALDI-2 imaging in analyzing endogenous lipids in CCS, which could potentially become powerful tools for future cancer studies.展开更多
Interfacial solar evaporation holds immense potential for brine desalination with low carbon footprints and high energy utilization.Hydrogels,as a tunable material platform from the molecular level to the macroscopic ...Interfacial solar evaporation holds immense potential for brine desalination with low carbon footprints and high energy utilization.Hydrogels,as a tunable material platform from the molecular level to the macroscopic scale,have been considered the most promising candidate for solar evaporation.However,the simultaneous achievement of high evaporation efficiency and satisfactory tolerance to salt ions in brine remains a challenging scientific bottleneck,restricting the widespread application.Herein,we report ionization engineering,which endows polymer chains of hydrogels with electronegativity for impeding salt ions and activating water molecules,fundamentally overcoming the hydrogel salt-impeded challenge and dramatically expediting water evaporating in brine.The sodium dodecyl benzene sulfonate-modified carbon black is chosen as the solar absorbers.The hydrogel reaches a ground-breaking evaporation rate of 2.9 kg m−2 h−1 in 20 wt%brine with 95.6%efficiency under one sun irradiation,surpassing most of the reported literature.More notably,such a hydrogel-based evaporator enables extracting clean water from oversaturated salt solutions and maintains durability under different high-strength deformation or a 15-day continuous operation.Meantime,on the basis of the cation selectivity induced by the electronegativity,we first propose an all-day system that evaporates during the day and generates salinity-gradient electricity using waste-evaporated brine at night,anticipating pioneer a new opportunity for all-day resource-generating systems in fields of freshwater and electricity.展开更多
Rydberg state excitation(RSE) is a highly non-linear physical phenomenon that is induced by the ionization of atoms or molecules in strong femtosecond laser fields. Here we observe that both parent and fragments(S, C,...Rydberg state excitation(RSE) is a highly non-linear physical phenomenon that is induced by the ionization of atoms or molecules in strong femtosecond laser fields. Here we observe that both parent and fragments(S, C, OC) of the triatomic molecule carbonyl sulfide(OCS) can survive strong 800 nm or 400 nm laser fields in high Rydberg states. The dependence of parent and fragment RSE yields on laser intensity and ellipticity is investigated in both laser fields, and the results are compared with those for strong-field ionization. Distinctly different tendencies for laser intensity and ellipticity are observed for fragment RSE compared with the corresponding ions. The mechanisms of RSE and strong-field ionization of OCS molecules in different laser fields are discussed based on the experimental results. Our study sheds some light on the strong-field excitation and ionization of molecules irradiated by femtosecond NIR and UV laser fields.展开更多
The mass application of Hall thrusters poses the need for a diagnostic method of ionization mechanism in the discharge channel to boost the iteration and optimization of thruster design.This work presents an Optical E...The mass application of Hall thrusters poses the need for a diagnostic method of ionization mechanism in the discharge channel to boost the iteration and optimization of thruster design.This work presents an Optical Emission Spectroscopy (OES) method for diagnostics of the contribution of different ionization mechanisms and the flux of ions in different valences in the discharge channel of a Hall thruster.The emission spectra in the discharge channel are analyzed by jointly utilizing a collisional-radiative model,an ionization-excitation model,and a flux-conservation model.It is found that the intensities of some spectral lines can be converted into the reaction rates of collision processes,e.g.,electron-induced excitation and ionization processes.The latter can further be used to determine the evolutions of particle fluxes by utilizing the conservation law of matter.The novel method is demonstrated on a kilo-watt Hall thruster.The evolutions of several parameters are determined using this method along the discharge channel,including the ionization rates of different mechanisms,particle fluxes,particle densities,and particle velocities.This novel method can be further developed by being jointly utilized with spectral imaging and tomography techniques,enabling diagnostics of multi-dimensional distributions of the above-mentioned parameters in the discharge channel and near-field plume.展开更多
We investigate propagation of dust ion acoustic solitary wave(DIASW)in a multicomponent dusty plasma with adiabatic ions,superthermal electrons,and stationary dust.The reductive perturbation method is employed to deri...We investigate propagation of dust ion acoustic solitary wave(DIASW)in a multicomponent dusty plasma with adiabatic ions,superthermal electrons,and stationary dust.The reductive perturbation method is employed to derive the damped Korteweg-de Vries(DKdV)equation which describes DIASW.The result reveals that the adiabaticity of ions significantly modifies the basic features of the DIASW.The ionization effect makes the solitary wave grow,while collisions reduce the growth rate and even lead to the damping.With the increases in ionization cross sectionΔσ/σ_(0),ion-to-electron density ratioδ_(ie)and superthermal electrons parameterκ,the effect of ionization on DIASW enhances.展开更多
The absolute partial and total cross sections for electron impact ionization of carbon monoxide are reported for electron energies from 350 eV to 8000 eV.The product ions(CO^(+),C^(+),O^(+),CO^(2+),C^(2+),and O^(2+))a...The absolute partial and total cross sections for electron impact ionization of carbon monoxide are reported for electron energies from 350 eV to 8000 eV.The product ions(CO^(+),C^(+),O^(+),CO^(2+),C^(2+),and O^(2+))are measured by employing an ion imaging mass spectrometer and two ion-pair dissociation channels(C^(+)+O^(+)and C^(2+)+O^(+))are identified.The absolute cross sections for producing individual ions and their total,as well as for the ion-pair dissociation channels are obtained by normalizing the data of CO^(+)to that of Ar^(+)from CO-Ar mixture target with a fixed 1:1 ratio.The overall errors are evaluated by considering various kinds of uncertainties.A comprehensive comparison is made with the available data,which shows a good agreement with each other over the energy ranges that are overlapped.This work presents new cross-section data with electron energies above 1000 eV.展开更多
The double ionization process of molecules driven by co-rotating two-color circularly polarized fields is investigated with a three-dimensional classical ensemble model. Numerical results indicate that a considerable ...The double ionization process of molecules driven by co-rotating two-color circularly polarized fields is investigated with a three-dimensional classical ensemble model. Numerical results indicate that a considerable part of the sequential double ionization(DI) events of molecules occur through internal collision double ionization(ICD), and the ICD recollision mechanism is significantly different from that in non-sequential double ionization(NSDI). By analyzing the results of internuclear distances R = 5 a.u. and 2 a.u., these two recollision mechanisms are studied in depth. It is found that the dynamic behaviors of the recollision mechanisms of NSDI and ICD are similar. For NSDI, the motion range of electrons after the ionization is relatively large, and the electrons will return to the core after a period of time. In the ICD process,electrons will rotate around the parent ion before ionization, and the distance of the electron motion is relatively small. After a period of time, the electrons will come back to the core and collide with another electron. Furthermore, the molecular internuclear distance has a significant effect on the electron dynamic behavior of the two ionization mechanisms. This study will help to understand the multi-electron ionization process of complex systems.展开更多
By numerically solving the two-dimensional(2D)time-dependent Schrödinger equation(TDSE),we present photoelectron momentum distributions(PMDs)and photoelectron angular distributions(PADs)of symmetric(H_(2)^(+))and...By numerically solving the two-dimensional(2D)time-dependent Schrödinger equation(TDSE),we present photoelectron momentum distributions(PMDs)and photoelectron angular distributions(PADs)of symmetric(H_(2)^(+))and asymmetric(HeH^(2+))molecular ions in circularly polarized(CP)laser pulses.By adjusting the laser wavelength,two circumstances of resonance excitation and direct ionization were considered.The ionization mechanism of the resonance excitation was mainly investigated.The results show that the PMDs of H_(2)^(+) and HeH^(2+) in the y-direction gradually increase with increasing intensity,and the number of PMDs lobes is in good agreement with the results predicted by the ultrafast ionization model.In the resonance excitation scenario,the PMDs of are dominated by two-photon ionization,whereas the PMDs of HeH_(2)^(+) are dominated by three-photon ionization.Furthermore,the PMDs of HeH^(2+)are stronger in the resonance excitation scenario than those of H_(2)^(+),which can be explained by the time-dependent population of electrons.In addition,the molecular structure is clearly imprinted onto the PMDs.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 National Key Research and Development Program of China(Grant No.2022YFE0134200)the National Natural Science Foundation of China(Grant Nos.12474343,12174147,and 12074142)the Natural Science Foundation of Jilin Province,China(Grant No.20220101016JC)。
文摘Strong feld-induced nonsequential double ionization(NSDI)is a signifcant multi-electron phenomenon that provides crucial insights into understanding electron correlation and multiple ionization of atoms and molecules,but it is typically unattainable in a circularly polarized laser pulse,especially for long-wavelength lasers.We present evidence that NSDI can occur in the presence of a near-infrared or beyond laser pulse by introducing a bowtie-nanotip.The laser-induced local plasmon can alter the local ellipticity of the feld,thereby enabling NSDI through elliptical trajectories that facilitate recollisions with parent atoms.An oval-shaped momentum distribution of recoiled ions provides evidence for the modifcation of trajectories by the aligned nanotips.Our study introduces an innovative control knob to manipulate NSDI and electron dynamics through the utilization of nanostructures.
基金supports by the National Natural Science Foundation of China(No.22174037)the Joint Funds of the Hunan Provincial Natural Science Foundation of China(No.2023JJ50255)+1 种基金Changsha Science and Technology Project(No.Z202269490128)National Key Research and Development Program of China(No.2023YFF0613400)are appreciated.
文摘Traditional electrospray ionization tandem mass spectrometry(ESI-MS^(n))has been a powerful tool in diverse research areas,however,it faces great limitations in the study of protein-small molecule interactions.In this article,the state-of-the-art temperature-controlled electrospray ionization tandem mass spectrometry(TC-ESI-MS^(n))is applied to investigate interactions between ubiquitin and two flavonol molecules,respectively.The combination of collision-induced dissociation(CID)and MS solution-melting experiments facilitates the understanding of flavonol-protein interactions in a new dimension across varying temperature ranges.While structural changes of proteins disturbed by small molecules are unseen in ESI-MS^(n),TC-ESI-MS^(n)allows a simultaneous assessment of the stability of the complex in both gas and liquid phases under various temperature conditions,meanwhile investigating the impact on the protein’s structure and tracking changes in thermodynamic data,and the characteristics of structural intermediates.
基金supported by Jiangxi Provincial International Science and Technology Cooperation Project(Nos.20203BDH80W010 and 20232BBH80012)the National Natural Science Foundation of China(Nos.82160410 and 81860379)+1 种基金Foundation of Jiangxi Provincial Department of Science and Technology(No.20212ACB206018)Key Research and Development Program of Jiangxi Province(No.20223BBG71009)。
文摘Accurate determination of lung cancer margins at the molecular level is of great significance to determine the optimal extent of resection during surgical operation and reduce the risk of postoperative recurrence.In this study,internal extractive electrospray ionization mass spectrometry(i EESI-MS)was used to trace potential molecular tumor margins in lung cancer tissue.Molecular differential model for the determination of lung cancer tumor margin was established via partial least-squares discriminant analysis(PLS-DA)of iEESI-MS data collected from lung tissue pieces within cancer tumor area and iEESI-MS data collected from lung tissue pieces outside cancer tumor area.Proof-of-concept data demonstrate that the developed molecular differential model yields ca.1-2 mm wider potential molecular tumor margin of a lung cancer compared to the conventional histological analysis,showing promising potential of iEESI-MS to increase the accuracy of tumor margins determination and lower risk of lung cancer postoperative recurrence.Furthermore,our results revealed that creatine and taurine showed positive correlations with lung cancer.
基金supported by the National Key R&D Program of China (Grant No. 2022YFF0503700)the special funds of Hubei Luojia Laboratory (220100011)+1 种基金Chao Xiong is supported by the ISSI-BJ project, “the electromagnetic data validation and scientific application research based on CSES satellite”ISSI/ISSI-BJ project “Multi-Scale Magnetosphere–Ionosphere–Thermosphere Interaction”。
文摘In this study, we provide a detailed case study of the X-pattern of equatorial ionization anomaly(EIA) observed on the night of September 12, 2021 by the Global-scale Observations of the Limb and Disk(GOLD) mission. Unlike most previous studies about the X-pattern observed under the severely disturbed background ionosphere, this event is observed under geomagnetically quiet and low solar activity conditions. GOLD's continuous observations reveal that the X-pattern intensity evolves with local time, while its center's longitude remains constant. The total electron content(TEC) data derived from the ground-based Global Navigation Satellite System(GNSS) network aligns well with GOLD observations in capturing the formation of the X-pattern, extending coverage to areas beyond GOLD's observational reach. Additionally, the ESA's Swarm mission show that both sides of the X-pattern can coincide with the occurrence of small-scale equatorial plasma bubbles(EPBs). To further analyze the possible drivers of the X-pattern, observations from the Ionospheric Connection Explorer(ICON) satellite were used. It shows that the latitudinal expansion(or width) between the EIA crests in two hemispheres is proportional(or inversely proportional) to the upward(or downward) plasma drift velocity, which suggests that the zonal electric field should have a notable influence on the formation of EIA X-pattern. Further simulations using the SAMI2 model support this mechanism, as the X-pattern of EIA is successfully reproduced by setting the vertical plasma drift to different values at different longitudes.
基金financially supported by Jiangxi University of Chinese Medicine School-level Science and Technology Innovation Team Development Program(No.CXTD22005)PhD research startup fund of Jiangxi University of Chinese Medicine(No.2023BSZR005)。
文摘Selenium is one of the important trace elements in the human body.Its deficiency will directly affect human health.With people's attention to health,the content of selenium in food has gradually attracted attention.However,detecting selenium compounds in complex samples remains a challenge.In this work,we built an online heating-reaction device.This device combines the electrospray extraction ionization mass spectrometry(EESI-MS)with the heating reaction device,which can simultaneously detect various selenium compounds in complex liquid samples.Under acidic conditions,the sample was heated and catalyzed by a heating reaction device,so that the SeO~(2-)_(3)and O-phenylenediamine(OPD)could generate 1,3-dihydro-2,1,3-benzoselenadiazole.Based on the above reactions,we can detect organic selenium,inorganic selenium and other compounds in liquid samples by organic mass spectrometry.In this experiment,we determined the content of three forms of selenium:selenomethionine(SeMet),l-selenocystine(SeCys(2)),and sodium selenite.The calibration curves for SeMet,SeCys(2),and sodium selenite showed strong linearity within a range of 0.50-50.00μg/L.The limits of detection(LOD)for the three compounds were 0.22,0.27,and 0.41μg/L,respectively.The limits of quantification(LOQ)were 0.68,0.81,and 1.23μg/L,respectively.Spiked recoveries at three levels ranged from 98.8%to 106.1%.In addition,this method can simultaneously detect three selenium compounds and three other specific chemical components in tea infusion samples,providing a rapid and efficient method for identifying tea quality.
基金supported by the National Natural Science Foundation of China (Nos. 12121004, 12274273, and 12450402)the Science and Technology Department of Hubei Province (No. 2020CFA029)+1 种基金CAS Project for Young Scientists in Basic Research (No. YSBR-091)the Youth Innovation Promotion Association CAS (No. 2021328)。
文摘The ultrafast excitation dynamics of atoms and molecules exposed to circularly polarized two-color(CPTC)laser fields constitute a fascinating topic in attosecond science. Although extensive research has established the relationship between the Rydberg state excitation(RSE) yields and the CPTC field parameters, such as field amplitude ratios and helicity of two components, the role of the relative phase(φ) in modulating RSE efficiency remains unclear. In this work, we theoretically investigate the φ dependence of RSE and ionization yields in the co-rotating and counter-rotating circularly polarized two-color(CPTC) few-cycle laser fields by a semiclassical model. We find that, in co-rotating CPTC fields, both RSE and ionization yields display pronounced oscillations as a function of φ and these oscillations are significantly suppressed in the counter-rotating configuration, particularly for ionization yields. Moreover, the ratio of RSE to ionization yields exhibits an out-of-phase oscillatory pattern between low-and high-intensity regimes. These results can be comprehended by the unique feature of φ dependence of CPTC few-cycle fields, based on our semiclassical analysis. Our results demonstrate that phase-controlled CPTC fields offer a versatile tool for steering ultrafast ionization and RSE dynamics of atoms and molecules.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12174239,12347165,and 12404330)Shaanxi Fundamental Science Research Project for Mathematics and Physics(Grant No.23JSY022)+2 种基金Natural Science Basic Research Program of Shaanxi(Grant No.2022JM-015)Hebei Natural Science Foundation(Grant No.A2022205002)Science and Technology Project of Hebei Education Department(Grant No.QN2022143)。
文摘This study analytically examines the ionization of atoms in strong near-circular laser fields.The classic Keldysh-Rutherford(KR)Coulomb-scattering(CS)model[Phys.Rev.Lett.121123201(2018)]successfully explained the attoclock experimental curve for the H atom at lower laser intensities.Here,we develop a semiclassical model that includes the initial conditions related to the quantum properties of tunneling in the KR model at the beginning of the scattering process.This model is able to explain recent attoclock experimental curves over a wider range of laser and atomic parameters.Our results show the importance of system symmetry and quantum effects in attoclock measurements,suggesting the complex role of the Coulomb potential in strong-field ionization.
基金Project supported by the Natural Science Foundation of Henan(Grant No.252300421304)the National Natural Science Foundation of China(Grant Nos.12204498,12474259+1 种基金12334011)the National Key Research and Development Program of China(Grant No.2022YFA1604302)。
文摘We propose a method to characterize the features of a cold strontium cloud in a magneto-optical trap(MOT)through the photoionization of cold Sr atoms in a custom-designed reaction microscope.Sr atoms in the dark state of 5s5p3P2 populated via the cascade transition 5s5p^(1)P_(1)→5s4d^(1)D_(2)→5s5p^(3)P_(2)accumulate a significant fraction,giving a long lifetime of 520 s.These atoms in the dark state are subsequently trapped by the gradient magnetic field of the MOT.By scanning the Sr+momentum distributions ionized with an 800 nm infrared femtosecond laser,we are able to outline the size of~0.55 mm in radius and the temperature of~0.40 mK for the dark-state atoms,which is significantly cooler than the MOT temperature of 3.3 mK trapped in the 461 nm.The size of MOT exhibits an oblate spheroidal distribution with a radius of approximately 0.35 mm and 0.55 mm,extracted with momenta of photoion and absorption imaging,respectively.The results using the photoion momenta are consistent with the expected results from absorption imaging,which confirms the method's reliability.The advantage of this method is the ability to simultaneously characterize the distribution information of atoms in different initial states within the cold atomic cloud.
基金supported by the National Key Research and Development Program of China(No.2022YFA1602502)the National Natural Science Foundation of China(No.12127804).
文摘The direct and dissociative ionizations of oxygen molecule are investigated experimen-tally by electron collision with energies from 350 eV to 8000 eV.The absolute ionization cross sections for the product ions(O_(2)^(2+),O_(2)^(2+)O^(+),O^(2+),and their total)and two Coulomb explosion channels(O^(+)+O^(+)and O^(2+)+O^(+))are obtained by putting the data of O^(2+)on the scale of Ar+from O_(2)and Ar gases mixed with a fixed relative flow ratio of 1:1.The experimental errors are assessed by taking uncertainties of various factors into account.The present absolute cross sections are well consistent with the previous data in the overlapped energy range below 1000 eV.
基金supported by the National Natural Science Foundation of China (Grant No. 12074329)Nanhu Scholars Program for Young Scholars of Xinyang Normal University。
文摘With a three-dimensional semiclassical ensemble method, we theoretically investigated the nonsequential double ionization of Ar driven by the spatially inhomogeneous few-cycle negatively chirped laser pulses. Our results show that the recollision time window can be precisely controlled within an isolated time interval of several hundred attoseconds, which is useful for understanding the subcycle correlated electron dynamics. More interestingly, the correlated electron momentum distribution (CEMD) exhibits a strong dependence on laser intensity. That is, at lower laser intensity, CEMD is located in the first quadrant. As the laser intensity increases,CEMD shifts almost completely to the second and fourth quadrants, and then gradually to the third quadrant.The underlying physics governing the CEMD's dependence on laser intensity is explained.
基金Project supported by the National Natural Science Foundation of China (Grant Nos.92150105,11834004,12227807,and 12241407)the Science and Technology Commission of Shanghai Municipality (Grant No.21ZR1420100)。
文摘Electronic processes within atoms and molecules reside on the timescale of attoseconds. Recent advances in the laserbased pump-probe interrogation techniques have made possible the temporal resolution of ultrafast electronic processes on the attosecond timescale, including photoionization and tunneling ionization. These interrogation techniques include the attosecond streak camera, the reconstruction of attosecond beating by interference of two-photon transitions, and the attoclock. While the former two are usually employed to study photoionization processes, the latter is typically used to investigate tunneling ionization. In this review, we briefly overview these timing techniques towards an attosecond temporal resolution of ionization processes in atoms and molecules under intense laser fields. In particular, we review the backpropagation method, which is a novel hybrid quantum-classical approach towards the full characterization of tunneling ionization dynamics. Continued advances in the interrogation techniques promise to pave the pathway towards the exploration of ever faster dynamical processes on an ever shorter timescale.
基金supported by the National Natural Science Foundation of China (Nos.22036001, 22276034 and 22106130)。
文摘Cancer cell spheroids(CCS) are a valuable three-dimensional cell model in cancer studies because they could replicate numerous characteristics of solid tumors. Increasing researches have used matrix-assisted laser desorption/ionization mass spectrometry imaging(MALDI-MSI) to investigate the spatial distribution of endogenous compounds(e.g., lipids) in CCS. However, only limited lipid species can be detected owing to a low ion yield by using MALDI. Besides, it is still challenging to fully characterize the structural diversity of lipids due to the existence of isomeric/isobaric species. Here, we carried out the initial application of MALDI coupled with laser-postionization(MALDI-2) and trapped ion mobility spectrometry(TIMS) imaging in HCT116 colon CCS to address these challenges. We demonstrated that MALDI-2 is capable of detecting more number and classes of lipids in HCT116 colon CCS with higher signal intensities than MALDI. TIMS could successfully separate numerous isobaric/isomeric species of lipids in CCS. Interestingly, we found that some isomeric/isobaric species have totally different spatial distributions in colon CCS. Further MS/MS imaging analysis was employed to determine the compositions of fatty acid chains for isomeric species by examining disparities in signal intensities and spatial distributions of product ions. This work stresses the robust ability of TIMS and MALDI-2 imaging in analyzing endogenous lipids in CCS, which could potentially become powerful tools for future cancer studies.
基金the National Natural Science Foundation of China(Grant No.52076028).
文摘Interfacial solar evaporation holds immense potential for brine desalination with low carbon footprints and high energy utilization.Hydrogels,as a tunable material platform from the molecular level to the macroscopic scale,have been considered the most promising candidate for solar evaporation.However,the simultaneous achievement of high evaporation efficiency and satisfactory tolerance to salt ions in brine remains a challenging scientific bottleneck,restricting the widespread application.Herein,we report ionization engineering,which endows polymer chains of hydrogels with electronegativity for impeding salt ions and activating water molecules,fundamentally overcoming the hydrogel salt-impeded challenge and dramatically expediting water evaporating in brine.The sodium dodecyl benzene sulfonate-modified carbon black is chosen as the solar absorbers.The hydrogel reaches a ground-breaking evaporation rate of 2.9 kg m−2 h−1 in 20 wt%brine with 95.6%efficiency under one sun irradiation,surpassing most of the reported literature.More notably,such a hydrogel-based evaporator enables extracting clean water from oversaturated salt solutions and maintains durability under different high-strength deformation or a 15-day continuous operation.Meantime,on the basis of the cation selectivity induced by the electronegativity,we first propose an all-day system that evaporates during the day and generates salinity-gradient electricity using waste-evaporated brine at night,anticipating pioneer a new opportunity for all-day resource-generating systems in fields of freshwater and electricity.
基金Project supported by the National Key Program for S&T Research and Development(Grant No.2019YFA0307700)the National Natural Science Foundation of China(Grant Nos.12174148,11874179,12074144,and 12074146)。
文摘Rydberg state excitation(RSE) is a highly non-linear physical phenomenon that is induced by the ionization of atoms or molecules in strong femtosecond laser fields. Here we observe that both parent and fragments(S, C, OC) of the triatomic molecule carbonyl sulfide(OCS) can survive strong 800 nm or 400 nm laser fields in high Rydberg states. The dependence of parent and fragment RSE yields on laser intensity and ellipticity is investigated in both laser fields, and the results are compared with those for strong-field ionization. Distinctly different tendencies for laser intensity and ellipticity are observed for fragment RSE compared with the corresponding ions. The mechanisms of RSE and strong-field ionization of OCS molecules in different laser fields are discussed based on the experimental results. Our study sheds some light on the strong-field excitation and ionization of molecules irradiated by femtosecond NIR and UV laser fields.
基金financially supported by the National Natural Science Foundation of China (No.U22B2094)。
文摘The mass application of Hall thrusters poses the need for a diagnostic method of ionization mechanism in the discharge channel to boost the iteration and optimization of thruster design.This work presents an Optical Emission Spectroscopy (OES) method for diagnostics of the contribution of different ionization mechanisms and the flux of ions in different valences in the discharge channel of a Hall thruster.The emission spectra in the discharge channel are analyzed by jointly utilizing a collisional-radiative model,an ionization-excitation model,and a flux-conservation model.It is found that the intensities of some spectral lines can be converted into the reaction rates of collision processes,e.g.,electron-induced excitation and ionization processes.The latter can further be used to determine the evolutions of particle fluxes by utilizing the conservation law of matter.The novel method is demonstrated on a kilo-watt Hall thruster.The evolutions of several parameters are determined using this method along the discharge channel,including the ionization rates of different mechanisms,particle fluxes,particle densities,and particle velocities.This novel method can be further developed by being jointly utilized with spectral imaging and tomography techniques,enabling diagnostics of multi-dimensional distributions of the above-mentioned parameters in the discharge channel and near-field plume.
基金supported by the Project of Scientific and Technological Innovation Base of Jiangxi Province,China (Grant No.20203CCD46008)the Key R&D Plan of Jiangxi Province,China (Grant No.20223BBH80006)+1 种基金the Natural Science Foundation of Jiangxi Province,China (Grant No.20212BAB211025)the Jiangxi Province Key Laboratory of Fusion and Information Control (Grant No.20171BCD40005)。
文摘We investigate propagation of dust ion acoustic solitary wave(DIASW)in a multicomponent dusty plasma with adiabatic ions,superthermal electrons,and stationary dust.The reductive perturbation method is employed to derive the damped Korteweg-de Vries(DKdV)equation which describes DIASW.The result reveals that the adiabaticity of ions significantly modifies the basic features of the DIASW.The ionization effect makes the solitary wave grow,while collisions reduce the growth rate and even lead to the damping.With the increases in ionization cross sectionΔσ/σ_(0),ion-to-electron density ratioδ_(ie)and superthermal electrons parameterκ,the effect of ionization on DIASW enhances.
基金Project supported by the National Key Research and Development Program of China (Grant No.2022YFA1602502)the National Natural Science Foundation of China (Grant No.12127804)the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant Nos.XDB34000000)。
文摘The absolute partial and total cross sections for electron impact ionization of carbon monoxide are reported for electron energies from 350 eV to 8000 eV.The product ions(CO^(+),C^(+),O^(+),CO^(2+),C^(2+),and O^(2+))are measured by employing an ion imaging mass spectrometer and two ion-pair dissociation channels(C^(+)+O^(+)and C^(2+)+O^(+))are identified.The absolute cross sections for producing individual ions and their total,as well as for the ion-pair dissociation channels are obtained by normalizing the data of CO^(+)to that of Ar^(+)from CO-Ar mixture target with a fixed 1:1 ratio.The overall errors are evaluated by considering various kinds of uncertainties.A comprehensive comparison is made with the available data,which shows a good agreement with each other over the energy ranges that are overlapped.This work presents new cross-section data with electron energies above 1000 eV.
基金the National Key Research and Development Program of China (Grant No.2019YFA0307700)the National Natural Science Foundation of China (Grant Nos.12074145 and 11975012)+1 种基金Jilin Provincial Research Foundation for Basic Research,China (Grant No.20220101003JC)Jilin Provincial Education Department (Grant No.JJKH20230284KJ)。
文摘The double ionization process of molecules driven by co-rotating two-color circularly polarized fields is investigated with a three-dimensional classical ensemble model. Numerical results indicate that a considerable part of the sequential double ionization(DI) events of molecules occur through internal collision double ionization(ICD), and the ICD recollision mechanism is significantly different from that in non-sequential double ionization(NSDI). By analyzing the results of internuclear distances R = 5 a.u. and 2 a.u., these two recollision mechanisms are studied in depth. It is found that the dynamic behaviors of the recollision mechanisms of NSDI and ICD are similar. For NSDI, the motion range of electrons after the ionization is relatively large, and the electrons will return to the core after a period of time. In the ICD process,electrons will rotate around the parent ion before ionization, and the distance of the electron motion is relatively small. After a period of time, the electrons will come back to the core and collide with another electron. Furthermore, the molecular internuclear distance has a significant effect on the electron dynamic behavior of the two ionization mechanisms. This study will help to understand the multi-electron ionization process of complex systems.
基金Project supported by the Natural Science Foundation of Jilin Province(Grant No.20220101010JC)the National Natural Science Foundation of China(Grant No.12074146)。
文摘By numerically solving the two-dimensional(2D)time-dependent Schrödinger equation(TDSE),we present photoelectron momentum distributions(PMDs)and photoelectron angular distributions(PADs)of symmetric(H_(2)^(+))and asymmetric(HeH^(2+))molecular ions in circularly polarized(CP)laser pulses.By adjusting the laser wavelength,two circumstances of resonance excitation and direct ionization were considered.The ionization mechanism of the resonance excitation was mainly investigated.The results show that the PMDs of H_(2)^(+) and HeH^(2+) in the y-direction gradually increase with increasing intensity,and the number of PMDs lobes is in good agreement with the results predicted by the ultrafast ionization model.In the resonance excitation scenario,the PMDs of are dominated by two-photon ionization,whereas the PMDs of HeH_(2)^(+) are dominated by three-photon ionization.Furthermore,the PMDs of HeH^(2+)are stronger in the resonance excitation scenario than those of H_(2)^(+),which can be explained by the time-dependent population of electrons.In addition,the molecular structure is clearly imprinted onto the PMDs.
