We study the above-threshold ionization(ATI)process of atoms exposed to fundamental and high-frequency lasers with arbitrary ellipticity by applying the frequency-domain theory.It is found that the angular-resolved AT...We study the above-threshold ionization(ATI)process of atoms exposed to fundamental and high-frequency lasers with arbitrary ellipticity by applying the frequency-domain theory.It is found that the angular-resolved ATI spectrum is sensitive to ellipticities of two lasers and emitted angles of the photoelectron.Particularly for the photon energy of the highfrequency laser more than atomic ionization potential,the width of plateau tends to a constant with increasing ellipticity of fundamental field,the dip structure disappears with increasing ellipticity of the high-frequency field.With the help of the quantum channel analysis,it is shown that the angular distribution depends mainly on the ellipticity of high-frequency field in the case that its frequency is high.Moreover,one can see that the maximal and minimal energies in quantum numerical results are in good agreement with the classical prediction.Our investigation may provide theoretical support for experimental research on polarization control of ionization in elliptically polarized two-color laser fields.展开更多
Above-threshold ionization （ATI） of a hydrogen atom exposed to chirped laser fields is investigated theoretically by solving the time-dependent Schrodinger equation. By comparing the energy spectra, the two-dimensio...Above-threshold ionization （ATI） of a hydrogen atom exposed to chirped laser fields is investigated theoretically by solving the time-dependent Schrodinger equation. By comparing the energy spectra, the two-dimensional momentum spectra, and the angular distributions of photoelectron for the laser pulses with different chirp rates, we show a very clear chirp dependence both in the multiphoton and tunneling ionization processes but no chirp dependence in the single-photon ionization. We find that the chirp dependence in the multiphoton ionization based ATI can be attributed to the excited bound states. In the single-photon and tunneling ionization regimes, the electron can be removed directly from the ground state and thus the excited states may not be very important. It indicates that the chirp dependence in the tunneling ionization based ATI processes is mainly due to the laser pulses with different chirp rates,展开更多
We investigate the low-energy structure （LES） in the above-threshold ionization spectrum at a mid-infrared laser wavelength with a semiclassical model. Using a softened Coulomb potential （CP） and changing the soft...We investigate the low-energy structure （LES） in the above-threshold ionization spectrum at a mid-infrared laser wavelength with a semiclassical model. Using a softened Coulomb potential （CP） and changing the softening parameter, we show that though the very low-energy structure （VLES） and high low-energy structure （HLES） are both due to the interaction between the ionic CP and the electron, the two structures have different physical mechanisms： the VLES can be attributed to the electron-ion Coulomb interaction at a rather small distance and the HLES is more likely to be ascribed to the electron-ion Coulomb interaction at a large distance.展开更多
Using the frequency-domain theory, we investigate the above-threshold ionization（ATI） process of an atom in twocolor laser fields. When both photon energies of the two-color laser fields are much smaller than the at...Using the frequency-domain theory, we investigate the above-threshold ionization（ATI） process of an atom in twocolor laser fields. When both photon energies of the two-color laser fields are much smaller than the atomic ionization threshold, the ATI spectrum depends on the angle between the two lasers＇ polarization directions. While when the photon energy of one laser is comparable with or larger than the atomic ionization threshold, the ATI spectrum is independent of the angle, and only several dips appear at certain angles. By analyzing the contributions of different quantum channels, we find that, for the case that both frequencies of the two color lasers are low, the quantum interferences between the channels are strong, and hence the spectrum changes with the angle between the two lasers＇ polarization directions. While for the case that the frequency of one of the two color lasers is high, the contributions of the channels to the ATI spectrum decrease dramatically with increasing channel order, hence the interferences between the channels disappear, and the ATI spectrum has a step-like structure, which is independent of the angle between the two lasers＇ polarizations. These results can shed light on the study of the corresponding relation between classical and quantum mechanisms of the matter–laser interaction in high-frequency laser fields.展开更多
Using the time-dependent pseudo-spectral scheme, we solve the time-dependent Schrodinger equation of a hydrogen- like atom in a strong laser field in momentum space. The intensity-resolved photoelectron energy spectru...Using the time-dependent pseudo-spectral scheme, we solve the time-dependent Schrodinger equation of a hydrogen- like atom in a strong laser field in momentum space. The intensity-resolved photoelectron energy spectrum in abovethreshold ionization is obtained and further analyzed. We find that with the increase of the laser intensity, the abovethreshold ionization emission spectrum exhibits periodic resonance structure. By analyzing the population of atomic bound states, we find that it is the multi-photon excitation of bound state that leads to the occurrence of this phenomenon, which is in fairly good agreement with the experimental results.展开更多
We investigate atomic above-threshold ionization in elliptically polarized strong laser fields with a semiclassical approach.With increasing laser intensity,the Coulomb focusing（CF） effects are found to become stron...We investigate atomic above-threshold ionization in elliptically polarized strong laser fields with a semiclassical approach.With increasing laser intensity,the Coulomb focusing（CF） effects are found to become stronger in both parallel and perpendicular directions with respect to the polarization plane.The dependence of CF effects on tunnel exit,initial transverse momentum distribution and laser electric field is analyzed.It was revealed that the effects of tunnel exit are most prominent with variation of the laser intensity,and the other two factors both play non-negligible roles.Our results provide a deeper insight to the recent experiments of Coulomb asymmetry[Shafir D,et al.,2013 Phys.Rev.Lett.111 023005 and Li M,et al,2013 Phys.Rev.Lett.111 023006].展开更多
We investigate the above-threshold ionization of an atom in a combined infrared （IR） and extreme ultraviolet （XUV） two-color laser field and focus on the role of XUV field in the high-order above-threshold ionizat...We investigate the above-threshold ionization of an atom in a combined infrared （IR） and extreme ultraviolet （XUV） two-color laser field and focus on the role of XUV field in the high-order above-threshold ionization （HATI） process. It is demonstrated that, in stark contrast to previous studies, the XUV laser may play a significant role in atomic HATI process, and in particular, the XUV laser can accelerate the ionized electron in a quantized way during the collision between the electron and its parent ion. This process cannot be explained by the elassical three-step model Our results indicate that the previously well-established concept that HATI is an elastic recollision process is broken down.展开更多
According to the frequency-domain theory, we investigate the asymmetric structure of above-threshold ionization(ATI) spectrum of an atom in two-color elliptically polarized(EP) laser fields. When both laser fields are...According to the frequency-domain theory, we investigate the asymmetric structure of above-threshold ionization(ATI) spectrum of an atom in two-color elliptically polarized(EP) laser fields. When both laser fields are linearly polarized(LP), the spectrum shows that the multi-plateau structure is symmetric about the emitted angle of electron at π/2, while the spectrum becomes asymmetric and shifts rightwards with the increase of the EP degree of the IR laser field. Since the total ATI process is regarded as including direct ATI and the rescattering ATI, we analyze the spectrum structure of direct ATI and rescattering ATI separately. Using the saddle-point approximation, we find that for direct ATI, the fringes on the spectrum are mainly attributed to the fact that the ionization probability becomes very small when the direction of emitted electrons is perpendicular to the direction of the XUV laser polarization;while for the rescattering ATI, the interference fringes on the spectrum mainly come from the superposition of the waist structures on the spectra of all sub-channels.展开更多
The direct above-threshold ionization(ATI) of diatomic molecules in linearly-polarized infrared and extreme ultraviolet(IR+XUV) laser fields is investigated by the frequency–domain theory based on the nonperturbative...The direct above-threshold ionization(ATI) of diatomic molecules in linearly-polarized infrared and extreme ultraviolet(IR+XUV) laser fields is investigated by the frequency–domain theory based on the nonperturbative quantum electrodynamics. The destructive interference fringes on the angle-resolved ATI spectra, which are closely related to the molecular structure, can be well fitted by a simple predictive formula for any alignment of the molecular axis. By comparing the direct ATI spectra for monochromatic and two-color laser fields, we found that the XUV laser field can both raise the ionization probability and the kinetic energy of the ionized electron, while the infrared(IR) laser field can broaden the energy distribution of the ionized electron. Our results demonstrate that, by using IR+XUV two-color laser fields, the angle-resolved spectra of the direct ATI can image the structural information of molecules without considering the recollision process of the ionized electron.展开更多
In this work, we mainly investigate the NH3 molecular multiphoton ionization process by using the photoelectron velocity map imaging technique. Under the condition of femtosecond laser(wavelength at 800 nm), the photo...In this work, we mainly investigate the NH3 molecular multiphoton ionization process by using the photoelectron velocity map imaging technique. Under the condition of femtosecond laser(wavelength at 800 nm), the photoelectron images are detected. The channel switching and above-threshold ionization(ATI) effect are also confirmed. The kinetic energy spectrum(KES) and the photoelectron angular distributions(PADs) are obtained through the anti-Abel transformation from the original images, and then three ionization channels are confirmed successfully according to the Freeman resonance effect in a relatively low laser intensity region. In the excitation process, the intermediate resonance Rydberg states are C^1 A 1(6 + 2 photons process), B^1 E(6 + 2 photons process) and C^1 A 1(7 + 2 photons process), respectively. At the same time, we also find that the photoelectron angular distributions are independent of laser intensity. In addition, the electrons produced by different processes interfere with each other and they can produce a spider-like structure. We also find ac-Stark movement according to the Stark-shift-induced resonance effect when the laser intensity is relatively high.展开更多
The high-resolution three-dimensional photoelectron momentum distributions via above-threshold ionization(ATI)of Xe atoms are measured in an intense near circularly polarized laser field using velocity map imaging and...The high-resolution three-dimensional photoelectron momentum distributions via above-threshold ionization(ATI)of Xe atoms are measured in an intense near circularly polarized laser field using velocity map imaging and tomography reconstruction. Compared to the linearly polarized laser field, the employed near circularly polarized laser field imposes a more strict selection rule for the transition via resonant excitation, and therefore we can selectively enhance the resonant ATI through certain atomic Rydberg states. Our results show the self-reference ionization delay, which is determined from the difference between the measured streaking angles for nonadiabatic ATI via the 4 f and 5 f Rydberg states, is 45.6 as. Our method provides an accessible route to highlight the role of resonant transition between selected states, which will pave the way for fully understanding the ionization dynamics toward manipulating electron motion as well as reaction in an ultrafast time scale.展开更多
The gauge problem of Keldysh-Faisal-Reiss theories is discussed.It is found that the E-gauge used by Keldysh is more reasonable than the A-gauge used by Reiss.The Keldysh theory is then developed further.Its different...The gauge problem of Keldysh-Faisal-Reiss theories is discussed.It is found that the E-gauge used by Keldysh is more reasonable than the A-gauge used by Reiss.The Keldysh theory is then developed further.Its differential ionization rate gives more hot electrons than Reiss's and therefore better agrees the experimental result.The another remarkable point is that the differential ionization rate as a function of energy is rapidly oscillatory.展开更多
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
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
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
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
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
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
In chemical science,the vertical ionization potential(VIP)is a crucial metric for understanding the electronegativity,hardness and softness of chemical material systems as well as the electronic structure and stabilit...In chemical science,the vertical ionization potential(VIP)is a crucial metric for understanding the electronegativity,hardness and softness of chemical material systems as well as the electronic structure and stability of molecules.Ever since the last century,the model chemistry composite methods have witnessed tremendous developments in computing the thermodynamic properties as well as the barrier heights.However,their performance in realm of the vertical electron processes of molecular systems has been rarely explored.In this study,we for the first time benchmarked the model chemistry composite methods(e.g.,CBS-QB3,G4 and W1BD)in comparison with the commonly used Koopmans's theorem(KT),electron propagator theory(e.g.,OVGF,D2,P3 and P3+)and CCSD(T)methods in calculating the VIP for up to 613 molecular systems with available experimental measurements.The large-scale test calculations strongly showed that the CBS-QB3 model chemistry composite technique can be well recommended to calculate VIP from the perspectives of accuracy,economy and applicability.Notably,the VIP values of up to 7 molecules were identified to have the absolute errors of larger than 0.3 e V at all calculation levels,which have strong hints that their VIP experimental values should be re-investigated.展开更多
基金Project supported by the National Natural Science Foundation of China (Grant Nos.12104285,12074240,12204135,12374260,12264013,12204136,92250303,and 12074418)the Guangdong Basicand Applied Basic Research Foundation (Grant No.2022A1515011742)+5 种基金the Special Scientific Research Program supported by the Shaanxi Education Department (Grant No.22JK0423)the Natural Science Basic Research Program of Shaanxi Province of China (Grant Nos.2023-JC-QN-0085 and 2023-JC-QN-0267)the Hainan Provincial Natural Science Foundation of China (Grant Nos.122CXTD504,123MS002,123QN179,123QN180,and 122QN217)the Sino-German Mobility Programme (Grant No.M-0031)the Xi’an Aeronautical Institute 2023 Innovation and Entrepreneurship Training Program for college students (Grant No.S202311736036)the Course Ideological and Political Education Program (Grant No.23ZLGC5030)。
文摘We study the above-threshold ionization(ATI)process of atoms exposed to fundamental and high-frequency lasers with arbitrary ellipticity by applying the frequency-domain theory.It is found that the angular-resolved ATI spectrum is sensitive to ellipticities of two lasers and emitted angles of the photoelectron.Particularly for the photon energy of the highfrequency laser more than atomic ionization potential,the width of plateau tends to a constant with increasing ellipticity of fundamental field,the dip structure disappears with increasing ellipticity of the high-frequency field.With the help of the quantum channel analysis,it is shown that the angular distribution depends mainly on the ellipticity of high-frequency field in the case that its frequency is high.Moreover,one can see that the maximal and minimal energies in quantum numerical results are in good agreement with the classical prediction.Our investigation may provide theoretical support for experimental research on polarization control of ionization in elliptically polarized two-color laser fields.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11664035,11465016,11764038,11364038,and 11564033)
文摘Above-threshold ionization （ATI） of a hydrogen atom exposed to chirped laser fields is investigated theoretically by solving the time-dependent Schrodinger equation. By comparing the energy spectra, the two-dimensional momentum spectra, and the angular distributions of photoelectron for the laser pulses with different chirp rates, we show a very clear chirp dependence both in the multiphoton and tunneling ionization processes but no chirp dependence in the single-photon ionization. We find that the chirp dependence in the multiphoton ionization based ATI can be attributed to the excited bound states. In the single-photon and tunneling ionization regimes, the electron can be removed directly from the ground state and thus the excited states may not be very important. It indicates that the chirp dependence in the tunneling ionization based ATI processes is mainly due to the laser pulses with different chirp rates,
基金Project supported by the National Natural Science Foundation of China (Grant Nos.10925420,11074026,11174330,and 11274050)the National Basic Research Program of China (Grant Nos.2011CB808102 and 2013CB922201)
文摘We investigate the low-energy structure （LES） in the above-threshold ionization spectrum at a mid-infrared laser wavelength with a semiclassical model. Using a softened Coulomb potential （CP） and changing the softening parameter, we show that though the very low-energy structure （VLES） and high low-energy structure （HLES） are both due to the interaction between the ionic CP and the electron, the two structures have different physical mechanisms： the VLES can be attributed to the electron-ion Coulomb interaction at a rather small distance and the HLES is more likely to be ascribed to the electron-ion Coulomb interaction at a large distance.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11474348 and 61275128)
文摘Using the frequency-domain theory, we investigate the above-threshold ionization（ATI） process of an atom in twocolor laser fields. When both photon energies of the two-color laser fields are much smaller than the atomic ionization threshold, the ATI spectrum depends on the angle between the two lasers＇ polarization directions. While when the photon energy of one laser is comparable with or larger than the atomic ionization threshold, the ATI spectrum is independent of the angle, and only several dips appear at certain angles. By analyzing the contributions of different quantum channels, we find that, for the case that both frequencies of the two color lasers are low, the quantum interferences between the channels are strong, and hence the spectrum changes with the angle between the two lasers＇ polarization directions. While for the case that the frequency of one of the two color lasers is high, the contributions of the channels to the ATI spectrum decrease dramatically with increasing channel order, hence the interferences between the channels disappear, and the ATI spectrum has a step-like structure, which is independent of the angle between the two lasers＇ polarizations. These results can shed light on the study of the corresponding relation between classical and quantum mechanisms of the matter–laser interaction in high-frequency laser fields.
基金Project supported by the National Basic Research Program of China(Grant No.2013CB922200)the National Natural Science Foundation of China(Grants Nos.11274141,11034003,11304116,11274001,and 11247024)the Jilin Provincial Research Foundation for Basic Research,China(Grant No.20140101168JC)
文摘Using the time-dependent pseudo-spectral scheme, we solve the time-dependent Schrodinger equation of a hydrogen- like atom in a strong laser field in momentum space. The intensity-resolved photoelectron energy spectrum in abovethreshold ionization is obtained and further analyzed. We find that with the increase of the laser intensity, the abovethreshold ionization emission spectrum exhibits periodic resonance structure. By analyzing the population of atomic bound states, we find that it is the multi-photon excitation of bound state that leads to the occurrence of this phenomenon, which is in fairly good agreement with the experimental results.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11547218,11564020,and 11504314)
文摘We investigate atomic above-threshold ionization in elliptically polarized strong laser fields with a semiclassical approach.With increasing laser intensity,the Coulomb focusing（CF） effects are found to become stronger in both parallel and perpendicular directions with respect to the polarization plane.The dependence of CF effects on tunnel exit,initial transverse momentum distribution and laser electric field is analyzed.It was revealed that the effects of tunnel exit are most prominent with variation of the laser intensity,and the other two factors both play non-negligible roles.Our results provide a deeper insight to the recent experiments of Coulomb asymmetry[Shafir D,et al.,2013 Phys.Rev.Lett.111 023005 and Li M,et al,2013 Phys.Rev.Lett.111 023006].
基金Supported by the National Natural Science Foundation of China under Grant Nos 11474348,61275128,11274050,11334009and 11425414the NSERC of Canada+1 种基金the Canadian Computing Facilities of SHARCnet and ACEnetthe National Basic Research Program of China under Grant No 2013CB922200
文摘We investigate the above-threshold ionization of an atom in a combined infrared （IR） and extreme ultraviolet （XUV） two-color laser field and focus on the role of XUV field in the high-order above-threshold ionization （HATI） process. It is demonstrated that, in stark contrast to previous studies, the XUV laser may play a significant role in atomic HATI process, and in particular, the XUV laser can accelerate the ionized electron in a quantized way during the collision between the electron and its parent ion. This process cannot be explained by the elassical three-step model Our results indicate that the previously well-established concept that HATI is an elastic recollision process is broken down.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11474348,11674198,11425414,and 11774411)
文摘According to the frequency-domain theory, we investigate the asymmetric structure of above-threshold ionization(ATI) spectrum of an atom in two-color elliptically polarized(EP) laser fields. When both laser fields are linearly polarized(LP), the spectrum shows that the multi-plateau structure is symmetric about the emitted angle of electron at π/2, while the spectrum becomes asymmetric and shifts rightwards with the increase of the EP degree of the IR laser field. Since the total ATI process is regarded as including direct ATI and the rescattering ATI, we analyze the spectrum structure of direct ATI and rescattering ATI separately. Using the saddle-point approximation, we find that for direct ATI, the fringes on the spectrum are mainly attributed to the fact that the ionization probability becomes very small when the direction of emitted electrons is perpendicular to the direction of the XUV laser polarization;while for the rescattering ATI, the interference fringes on the spectrum mainly come from the superposition of the waist structures on the spectra of all sub-channels.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11334009,11425414,11474348,and 11774411)
文摘The direct above-threshold ionization(ATI) of diatomic molecules in linearly-polarized infrared and extreme ultraviolet(IR+XUV) laser fields is investigated by the frequency–domain theory based on the nonperturbative quantum electrodynamics. The destructive interference fringes on the angle-resolved ATI spectra, which are closely related to the molecular structure, can be well fitted by a simple predictive formula for any alignment of the molecular axis. By comparing the direct ATI spectra for monochromatic and two-color laser fields, we found that the XUV laser field can both raise the ionization probability and the kinetic energy of the ionized electron, while the infrared(IR) laser field can broaden the energy distribution of the ionized electron. Our results demonstrate that, by using IR+XUV two-color laser fields, the angle-resolved spectra of the direct ATI can image the structural information of molecules without considering the recollision process of the ionized electron.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11574116,11534004,10704028,and 11474123)
文摘In this work, we mainly investigate the NH3 molecular multiphoton ionization process by using the photoelectron velocity map imaging technique. Under the condition of femtosecond laser(wavelength at 800 nm), the photoelectron images are detected. The channel switching and above-threshold ionization(ATI) effect are also confirmed. The kinetic energy spectrum(KES) and the photoelectron angular distributions(PADs) are obtained through the anti-Abel transformation from the original images, and then three ionization channels are confirmed successfully according to the Freeman resonance effect in a relatively low laser intensity region. In the excitation process, the intermediate resonance Rydberg states are C^1 A 1(6 + 2 photons process), B^1 E(6 + 2 photons process) and C^1 A 1(7 + 2 photons process), respectively. At the same time, we also find that the photoelectron angular distributions are independent of laser intensity. In addition, the electrons produced by different processes interfere with each other and they can produce a spider-like structure. We also find ac-Stark movement according to the Stark-shift-induced resonance effect when the laser intensity is relatively high.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11574101,11674116,11774111,and 11934006)the Open Fund of Hubei Provincial Key Laboratory of Optical Information and Pattern Recognition(Grant No.201902)the International Cooperation Program of Hubei Innovation Fund(Grant No.2019AHB052)。
文摘The high-resolution three-dimensional photoelectron momentum distributions via above-threshold ionization(ATI)of Xe atoms are measured in an intense near circularly polarized laser field using velocity map imaging and tomography reconstruction. Compared to the linearly polarized laser field, the employed near circularly polarized laser field imposes a more strict selection rule for the transition via resonant excitation, and therefore we can selectively enhance the resonant ATI through certain atomic Rydberg states. Our results show the self-reference ionization delay, which is determined from the difference between the measured streaking angles for nonadiabatic ATI via the 4 f and 5 f Rydberg states, is 45.6 as. Our method provides an accessible route to highlight the role of resonant transition between selected states, which will pave the way for fully understanding the ionization dynamics toward manipulating electron motion as well as reaction in an ultrafast time scale.
基金Supported by the National Natural Science Foundation of ChinaScience Foundation of China Academy of Engineering Physics.
文摘The gauge problem of Keldysh-Faisal-Reiss theories is discussed.It is found that the E-gauge used by Keldysh is more reasonable than the A-gauge used by Reiss.The Keldysh theory is then developed further.Its differential ionization rate gives more hot electrons than Reiss's and therefore better agrees the experimental result.The another remarkable point is that the differential ionization rate as a function of energy is rapidly oscillatory.
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 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funded by the National Natural Science Foundation of China(Nos.22073069,21773082)Science Research Project of Hebei Education Department(No.QN2024255)。
文摘In chemical science,the vertical ionization potential(VIP)is a crucial metric for understanding the electronegativity,hardness and softness of chemical material systems as well as the electronic structure and stability of molecules.Ever since the last century,the model chemistry composite methods have witnessed tremendous developments in computing the thermodynamic properties as well as the barrier heights.However,their performance in realm of the vertical electron processes of molecular systems has been rarely explored.In this study,we for the first time benchmarked the model chemistry composite methods(e.g.,CBS-QB3,G4 and W1BD)in comparison with the commonly used Koopmans's theorem(KT),electron propagator theory(e.g.,OVGF,D2,P3 and P3+)and CCSD(T)methods in calculating the VIP for up to 613 molecular systems with available experimental measurements.The large-scale test calculations strongly showed that the CBS-QB3 model chemistry composite technique can be well recommended to calculate VIP from the perspectives of accuracy,economy and applicability.Notably,the VIP values of up to 7 molecules were identified to have the absolute errors of larger than 0.3 e V at all calculation levels,which have strong hints that their VIP experimental values should be re-investigated.
