Abiotic oxygen formation predates photosynthesis,sustaining early chemical evolution,yet its elementary mechanisms remain contested.Here,we show the production pathways for molecular oxygen from doubly ionized carbon ...Abiotic oxygen formation predates photosynthesis,sustaining early chemical evolution,yet its elementary mechanisms remain contested.Here,we show the production pathways for molecular oxygen from doubly ionized carbon dioxide upon electron-impact.Through fragment ions and electron coincidence momentum imaging,we unambiguously determine the ionization mechanism by measuring the projectile energy loss in association with the C^(+) +O_(2)^(+) channel.Further potential energy and trajectory calculations enable us to elucidate the dynamical details of this fragmentation process,in which a bond rearrangement pathway is found to proceed via the structural deformation to a triangular intermediate.Moreover,we demonstrate a further roaming pathway for the formation of O_(2)^(+) from CO_(2)^(+) 2,in which a frustrated C-O bond cleavage leaves the O atom without sufficient energy to escape.The O atom then wanders around varied configuration spaces of the flat potential energy regions and forms a C-O-O_(2)^(+) intermediate prior to the final products C^(+) +O_(2)^(+).Considering the large quantities of free electrons in interstellar space,the processes revealed here are expected to be significant and should be incorporated into atmospheric evolution models.展开更多
The development of collinear resonance ionization spectroscopy for studying the nuclear structure of nickel isotopes far from the stability line relies on high-efficiency two-color two-step photoionization pathways.We...The development of collinear resonance ionization spectroscopy for studying the nuclear structure of nickel isotopes far from the stability line relies on high-efficiency two-color two-step photoionization pathways.We systematically investigated the even-parity autoionization spectrum of atomic nickel through resonance ionization mass spectrometry(RIMS).Fifteen intense single-color photoionization lines and corresponding transitions in the 300-325 nm range were identified and excluded as potential interference peaks for subsequent two-color studies.Fifty-one even-parity autoionization states in the 64000-66800 cm^(-1)range were identified for the first time by scanning from five intermediate excited states of the3d^(8)(^(3)F)4s4p(^(3)P^(o))configuration.Forty-eight of these states were assigned unique total angular momentum quantum numbers(J)based on electric dipole transition selection rules.The autoionization state at 64437.77 cm^(-1)was identified as an optimal final state for enhancing photoionization efficiency in two-color two-step pathways.This study provides comprehensive datasets of even-parity autoionization states of nickel,supporting both the advancement of collinear resonance ionization spectroscopy for exotic nickel isotopes and theoretical modeling of autoionization states.The datasets are openly available at https://doi.org/10.57760/sciencedb.j00113.00280.展开更多
We theoretically study the photoelectron momentum distributions from multiphoton ionization of a model lithium atom over a range of laser wavelengths from 500 nm to 700 nm by numerically solving the time-dependent Sch...We theoretically study the photoelectron momentum distributions from multiphoton ionization of a model lithium atom over a range of laser wavelengths from 500 nm to 700 nm by numerically solving the time-dependent Schr ¨odinger equation. The photoelectron momentum distributions display many ring-like patterns for the three-photon ionization, which vary dramatically with the change of the laser wavelength. We show that the wavelength-dependent photoelectron energy spectrum can be used to effectively identify the resonant and nonresonant ionization pathways. We also find an abnormal ellipticity dependence of the electron yield for the(2+1) resonance-enhanced ionization via the 4d intermediate state, which is relevant to the two-photon excitation probability from the ground state to the 4d state.展开更多
We study the ionization probabilities of atoms by a short laser pulse with three different theoretical methods, i.e., the numerical solution of the time-dependent SchrSdinger equation （TDSE）, the Perelomov-Popov Ter...We study the ionization probabilities of atoms by a short laser pulse with three different theoretical methods, i.e., the numerical solution of the time-dependent SchrSdinger equation （TDSE）, the Perelomov-Popov Terent＇ev （PPT） theory, and the Ammosov-Delone-Krainov （ADK） theory. Our results show that laser intensity dependent ionization probabilities of several atoms （i.e., H, He, and Ne） obtained from the PPT theory accord quite well with the TDSE results both in the multiphoton and tunneling ionization regimes, while the ADK results fit well to the TDSE data only in the tunneling ionization regime. Our calculations also show that laser intensity dependent ionization probabilities of a H atom at three different laser wavelengths of 600 nm, 800 nm, and 1200 nm obtained from the PPT theory are also in good agreement with those from the TDSE, while the ADK theory fails to give the wavelength dependence of ionization probability. Only when the laser wavelength is long enough, will the results of ADK be close to those of TDSE.展开更多
The elaborate energy and momentum spectra of ionized electrons from atoms in laser fields suggest that the ionization dynamics described by tunneling theory should be modified. Although great efforts have been carried...The elaborate energy and momentum spectra of ionized electrons from atoms in laser fields suggest that the ionization dynamics described by tunneling theory should be modified. Although great efforts have been carried out within semiclassical models, there are few discussions describing the multiphoton absorption process within a quantum framework. Comparing the results obtained with the time-dependent Schr?dinger equation(TDSE)and the Keldysh–Faisal–Reiss(KFR) theory, we study the nonperturbative effects of ionization dynamics beyond the KFR theory. The difference in momentum spectra between multiphoton and tunneling regimes is understood in a unified picture with virtual multiphoton absorption processes. For the multiphoton regime, the momentum spectra can be obtained by coherent interference of each periodic contribution. However, the interference of multiphoton absorption peaks will result in a complex structure of virtual multiphoton bands in the tunneling regime. It is shown that the virtual spectra will be almost continuous in the tunneling regime instead of the discrete levels found in the multiphoton regime. Finally, with a model combining the TDSE and the KFR theory,we try to understand the different effects of virtual multiphoton processes on ionization dynamics.展开更多
Using the numerical solution of the time-dependent SchrSdinger equation of a one-dimensional model atom in a two-colour laser field, we have investigated the effects of the potential models on coherent control of atom...Using the numerical solution of the time-dependent SchrSdinger equation of a one-dimensional model atom in a two-colour laser field, we have investigated the effects of the potential models on coherent control of atomic multiphoton ionization. It is found that the photoelectron spectra are obviously different for the long-range （Coulomb-like） and short-range （with no excited bound states） potential model atoms, which are produced by two-colour coherent control of atomic multiphoton ionization in a few laser cycles. Our results indicate that two-colour coherent control of atomic multiphoton ionization can be observed in simulations, depending on the choice of the model potentials.展开更多
This paper studies the multiphoton resonant ionization by two-colour laser pulses in the hydrogen atom by solving the time-dependent Schroedinger equation. By fixing the parameters of fundamental laser field and scann...This paper studies the multiphoton resonant ionization by two-colour laser pulses in the hydrogen atom by solving the time-dependent Schroedinger equation. By fixing the parameters of fundamental laser field and scanning the frequency of second laser field, it finds that the ionization probability shows several resonance peaks and is also much larger than the linear superposition of probabilities by applying two lasers separately. The enhancement of the ionization happens when the system is resonantly pumped to the excited states by absorbing two or more colour photons non-sequentially.展开更多
This paper studies the multiphoton ionization of the hydrogen atom exposed to the linearly or circularly polarized laser pulses by solving the time-dependent SchrSdinger equation. It finds that the ratio of the ioniza...This paper studies the multiphoton ionization of the hydrogen atom exposed to the linearly or circularly polarized laser pulses by solving the time-dependent SchrSdinger equation. It finds that the ratio of the ionization probabilities by linearly and circularly polarized laser pulses varies with the numbers of absorbing photons. With the same laser intensity, the circularly polarized laser pulse favors to ionize the atom with more ease than the linearly polarized laser pulse if only two or three photons are necessary to be absorbed. For the higher order multiphoton ionization, the linearly polarized laser pulse has the advantage over circularly polarized laser pulse to ionize the atom.展开更多
Multiply charged ions of Ar and NO were observed in MPI experiment Of NO/Ar with TOF-MS. A delayable pulsed acceleration field wn applied tO investigate the effect of the photoelectrons on the formation of the multi...Multiply charged ions of Ar and NO were observed in MPI experiment Of NO/Ar with TOF-MS. A delayable pulsed acceleration field wn applied tO investigate the effect of the photoelectrons on the formation of the multiply charged ions. The multiply charged ions were suggested to be produced by photoelectron impact ionization, in the region bentween the extractor grid and the repeller plate, step by step, from neutral species and lower charged ions. The 50-60ns of FWHM of the ion peaks implies that the pulse width of the photoelectrons should be shorter considering the broadening effect during the ionization process.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
We study the multiphoton ionization of potassium atoms in 800 nm and 400 nm femtosecond laser fields.In the 800 nm laser field,the potassium atom absorbs three photons and emits one electron via one photon resonance w...We study the multiphoton ionization of potassium atoms in 800 nm and 400 nm femtosecond laser fields.In the 800 nm laser field,the potassium atom absorbs three photons and emits one electron via one photon resonance with the 4p intermediate state with the help of the ac-Stark shift.The resonance feature is clearly shown as an Autler-Townes(AT) splitting and is mapped out in the electron kinetic energy spectrum.In a 400 nm laser field,although one photon resonance is possible with the 5p state,no splitting is observed.The different transition amplitudes between 4s-4p and 4s-5p explain the observed results.Due to the AT effect,an unexpected peak in the photoelectron energy spectrum that violates the dipole transition rule is observed.A preliminary explanation involving the spin-orbit interaction in the p state is given to account for this component.The observed ATsplitting in the electron kinetic energy distribution can be used as an effective method to calibrate the intensity of a laser field.展开更多
A simple low-cost system for detection of polycyclic aromatic hydrocarbon (PAH) in solution based on multiphoton ionization configuration is designed using a circulating ionization cell of 0.1 × 2 × 5 mm dim...A simple low-cost system for detection of polycyclic aromatic hydrocarbon (PAH) in solution based on multiphoton ionization configuration is designed using a circulating ionization cell of 0.1 × 2 × 5 mm dimension with quartz optical window. Fourth harmonic emission of Nd:YAG laser (266 nm, 6 ns, 10 Hz, and 2 mJ) and second harmonic generation of distributed feedback dye laser (278 - 286 nm, 20 ps, 10 Hz, and 300 μJ) were used as the ionization source. A high voltage of 800 V was applied to separate the ions after ionization. The photocurrent includes a sharp peak and a broad tail indexed to electron and ion currents, respectively. The lowest concentration of anthraxcene (C14H10) in order of few nano-grams per milliliter was detected by this multiphoton ionization configuration.展开更多
A fully quantum nonperturbative method is developed to describe multiphoton ionization in intense fields. It is shown that, treating the radiation field with quantum electrodynamic(QED) theory enables u s to obtain th...A fully quantum nonperturbative method is developed to describe multiphoton ionization in intense fields. It is shown that, treating the radiation field with quantum electrodynamic(QED) theory enables u s to obtain the above-threshold ionization energy distribution spectrum in analytical form firstly. Moreover, in addition to the well-known semiclassical theory, the framework presented here, derived from a QED perspective, provides a new picture of the multiphoton 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
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
Late-stage modification of complex molecules via site-selective hydrodefluorination is a challenging endeavor.The selective activation of carbon-fluorine(C-F) bonds in the presence of multiple C-F bonds is of importan...Late-stage modification of complex molecules via site-selective hydrodefluorination is a challenging endeavor.The selective activation of carbon-fluorine(C-F) bonds in the presence of multiple C-F bonds is of importance in organic synthesis and drug discovery.Herein,we describe the activation of C-F bonds via multiphoton photoredox catalysis to selectively produces a series of hydrodefluorinated compounds by simply tuning the reaction conditions.Moreover,this protocol was successfully applied to the late-stage functionalization of different drug-derivatives and the corresponding mono-,di-,and tri-defluorinated products were obtained in good to excellent yields.A detailed mechanistic investigation provides insight into the unprecedented hydrodefluorination pathway.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
The designing and manufacturing of micro/nanoscale tools for delivery,diagnostic,and therapeutic are essential for their multiscale integration in the precision medicine field.Conventional three-dimensional(3D)printin...The designing and manufacturing of micro/nanoscale tools for delivery,diagnostic,and therapeutic are essential for their multiscale integration in the precision medicine field.Conventional three-dimensional(3D)printing approaches are not suitable for such kind of tools due to the accuracy limitation.Multiphoton polymerization(MPP)-based micro/nanomanufacturing is a noncontact,high-precision molding technology that has been widely used in the micro/nano field is a promising tool for micro/nanoscale related precision medicine.In this article the fundamentals of MPP-based technology and the required materials in precision medicine are overviewed.The biomedical applications in various scenarios are then summarized and categorized as delivery systems,microtissue modeling,surgery,and diagnosis.Finally,the existing challenges and future perspectives on MPP-based micro/nanomanufacturing for precision medicine are discussed,focusing on material design,process optimization,and practical applications to overcome its current limitations.展开更多
基金supported by the National Natural Science Foundation of China (Grant Nos.12325406,92261201,12404305,and W2512072)the Shaanxi Province Natural Science Fundamental Research Project (Grant Nos.2023JC-XJ-03 and23JSQ013)the China Postdoctoral Science Foundation (Grant Nos.BX20240286 and 2024M7625)。
文摘Abiotic oxygen formation predates photosynthesis,sustaining early chemical evolution,yet its elementary mechanisms remain contested.Here,we show the production pathways for molecular oxygen from doubly ionized carbon dioxide upon electron-impact.Through fragment ions and electron coincidence momentum imaging,we unambiguously determine the ionization mechanism by measuring the projectile energy loss in association with the C^(+) +O_(2)^(+) channel.Further potential energy and trajectory calculations enable us to elucidate the dynamical details of this fragmentation process,in which a bond rearrangement pathway is found to proceed via the structural deformation to a triangular intermediate.Moreover,we demonstrate a further roaming pathway for the formation of O_(2)^(+) from CO_(2)^(+) 2,in which a frustrated C-O bond cleavage leaves the O atom without sufficient energy to escape.The O atom then wanders around varied configuration spaces of the flat potential energy regions and forms a C-O-O_(2)^(+) intermediate prior to the final products C^(+) +O_(2)^(+).Considering the large quantities of free electrons in interstellar space,the processes revealed here are expected to be significant and should be incorporated into atmospheric evolution models.
基金supported by the China National Nuclear Corporation Basic Research Project(Grant No.CNNC-JCYJ-202327)。
文摘The development of collinear resonance ionization spectroscopy for studying the nuclear structure of nickel isotopes far from the stability line relies on high-efficiency two-color two-step photoionization pathways.We systematically investigated the even-parity autoionization spectrum of atomic nickel through resonance ionization mass spectrometry(RIMS).Fifteen intense single-color photoionization lines and corresponding transitions in the 300-325 nm range were identified and excluded as potential interference peaks for subsequent two-color studies.Fifty-one even-parity autoionization states in the 64000-66800 cm^(-1)range were identified for the first time by scanning from five intermediate excited states of the3d^(8)(^(3)F)4s4p(^(3)P^(o))configuration.Forty-eight of these states were assigned unique total angular momentum quantum numbers(J)based on electric dipole transition selection rules.The autoionization state at 64437.77 cm^(-1)was identified as an optimal final state for enhancing photoionization efficiency in two-color two-step pathways.This study provides comprehensive datasets of even-parity autoionization states of nickel,supporting both the advancement of collinear resonance ionization spectroscopy for exotic nickel isotopes and theoretical modeling of autoionization states.The datasets are openly available at https://doi.org/10.57760/sciencedb.j00113.00280.
基金supported by National Key Research and Development Program of China (Grant No. 2019YFA0308300)the National Natural Science Foundation of China (Grant Nos. 12021004 and 61475055)。
文摘We theoretically study the photoelectron momentum distributions from multiphoton ionization of a model lithium atom over a range of laser wavelengths from 500 nm to 700 nm by numerically solving the time-dependent Schr ¨odinger equation. The photoelectron momentum distributions display many ring-like patterns for the three-photon ionization, which vary dramatically with the change of the laser wavelength. We show that the wavelength-dependent photoelectron energy spectrum can be used to effectively identify the resonant and nonresonant ionization pathways. We also find an abnormal ellipticity dependence of the electron yield for the(2+1) resonance-enhanced ionization via the 4d intermediate state, which is relevant to the two-photon excitation probability from the ground state to the 4d state.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 11044007,11164025,and 11064013)the Specialized Research Fund for the Doctoral Program of Higher Education of China (Grant Nos.20096203110001 and 20116203120001)the Foundation of Northwest Normal University,China (Grant No. NWNU-KJCXGC-03-62)
文摘We study the ionization probabilities of atoms by a short laser pulse with three different theoretical methods, i.e., the numerical solution of the time-dependent SchrSdinger equation （TDSE）, the Perelomov-Popov Terent＇ev （PPT） theory, and the Ammosov-Delone-Krainov （ADK） theory. Our results show that laser intensity dependent ionization probabilities of several atoms （i.e., H, He, and Ne） obtained from the PPT theory accord quite well with the TDSE results both in the multiphoton and tunneling ionization regimes, while the ADK results fit well to the TDSE data only in the tunneling ionization regime. Our calculations also show that laser intensity dependent ionization probabilities of a H atom at three different laser wavelengths of 600 nm, 800 nm, and 1200 nm obtained from the PPT theory are also in good agreement with those from the TDSE, while the ADK theory fails to give the wavelength dependence of ionization probability. Only when the laser wavelength is long enough, will the results of ADK be close to those of TDSE.
基金the National Natural Science Foundation of China under Grant Nos 11725417 and 11575027the Joint Fund of the National Natural Science Foundation of China and the China Academy of Engineering Physics under Grant No U1730449,and the Science Challenge Project under Grant No TZ2018005
文摘The elaborate energy and momentum spectra of ionized electrons from atoms in laser fields suggest that the ionization dynamics described by tunneling theory should be modified. Although great efforts have been carried out within semiclassical models, there are few discussions describing the multiphoton absorption process within a quantum framework. Comparing the results obtained with the time-dependent Schr?dinger equation(TDSE)and the Keldysh–Faisal–Reiss(KFR) theory, we study the nonperturbative effects of ionization dynamics beyond the KFR theory. The difference in momentum spectra between multiphoton and tunneling regimes is understood in a unified picture with virtual multiphoton absorption processes. For the multiphoton regime, the momentum spectra can be obtained by coherent interference of each periodic contribution. However, the interference of multiphoton absorption peaks will result in a complex structure of virtual multiphoton bands in the tunneling regime. It is shown that the virtual spectra will be almost continuous in the tunneling regime instead of the discrete levels found in the multiphoton regime. Finally, with a model combining the TDSE and the KFR theory,we try to understand the different effects of virtual multiphoton processes on ionization dynamics.
基金Project supported by the National Natural Science Foundation of China （Grant No 10674112） and the Young Teachers Foundation of Northwest Normal University （Grant No NWNU-QN-04-25）.
文摘Using the numerical solution of the time-dependent SchrSdinger equation of a one-dimensional model atom in a two-colour laser field, we have investigated the effects of the potential models on coherent control of atomic multiphoton ionization. It is found that the photoelectron spectra are obviously different for the long-range （Coulomb-like） and short-range （with no excited bound states） potential model atoms, which are produced by two-colour coherent control of atomic multiphoton ionization in a few laser cycles. Our results indicate that two-colour coherent control of atomic multiphoton ionization can be observed in simulations, depending on the choice of the model potentials.
基金supports by the Beijing Key Laboratory for Nano-Photonics and Nano-Structure
文摘This paper studies the multiphoton resonant ionization by two-colour laser pulses in the hydrogen atom by solving the time-dependent Schroedinger equation. By fixing the parameters of fundamental laser field and scanning the frequency of second laser field, it finds that the ionization probability shows several resonance peaks and is also much larger than the linear superposition of probabilities by applying two lasers separately. The enhancement of the ionization happens when the system is resonantly pumped to the excited states by absorbing two or more colour photons non-sequentially.
基金supports by the Beijing Key Laboratory for Nano-Photonics and Nano-Structure
文摘This paper studies the multiphoton ionization of the hydrogen atom exposed to the linearly or circularly polarized laser pulses by solving the time-dependent SchrSdinger equation. It finds that the ratio of the ionization probabilities by linearly and circularly polarized laser pulses varies with the numbers of absorbing photons. With the same laser intensity, the circularly polarized laser pulse favors to ionize the atom with more ease than the linearly polarized laser pulse if only two or three photons are necessary to be absorbed. For the higher order multiphoton ionization, the linearly polarized laser pulse has the advantage over circularly polarized laser pulse to ionize the atom.
文摘Multiply charged ions of Ar and NO were observed in MPI experiment Of NO/Ar with TOF-MS. A delayable pulsed acceleration field wn applied tO investigate the effect of the photoelectrons on the formation of the multiply charged ions. The multiply charged ions were suggested to be produced by photoelectron impact ionization, in the region bentween the extractor grid and the repeller plate, step by step, from neutral species and lower charged ions. The 50-60ns of FWHM of the ion peaks implies that the pulse width of the photoelectrons should be shorter considering the broadening effect during the ionization process.
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Supported by the National Key R&D Program of China (Grant No.2019YFA0307701)the National Natural Science Foundation of China (Grant Nos.91850114,11774131,12074143,11704148,11704147,and 11904120)+1 种基金the Science Challenge Project (Grant No.TZ2018005)the finical support of the starting grant from Jilin University。
文摘We study the multiphoton ionization of potassium atoms in 800 nm and 400 nm femtosecond laser fields.In the 800 nm laser field,the potassium atom absorbs three photons and emits one electron via one photon resonance with the 4p intermediate state with the help of the ac-Stark shift.The resonance feature is clearly shown as an Autler-Townes(AT) splitting and is mapped out in the electron kinetic energy spectrum.In a 400 nm laser field,although one photon resonance is possible with the 5p state,no splitting is observed.The different transition amplitudes between 4s-4p and 4s-5p explain the observed results.Due to the AT effect,an unexpected peak in the photoelectron energy spectrum that violates the dipole transition rule is observed.A preliminary explanation involving the spin-orbit interaction in the p state is given to account for this component.The observed ATsplitting in the electron kinetic energy distribution can be used as an effective method to calibrate the intensity of a laser field.
文摘A simple low-cost system for detection of polycyclic aromatic hydrocarbon (PAH) in solution based on multiphoton ionization configuration is designed using a circulating ionization cell of 0.1 × 2 × 5 mm dimension with quartz optical window. Fourth harmonic emission of Nd:YAG laser (266 nm, 6 ns, 10 Hz, and 2 mJ) and second harmonic generation of distributed feedback dye laser (278 - 286 nm, 20 ps, 10 Hz, and 300 μJ) were used as the ionization source. A high voltage of 800 V was applied to separate the ions after ionization. The photocurrent includes a sharp peak and a broad tail indexed to electron and ion currents, respectively. The lowest concentration of anthraxcene (C14H10) in order of few nano-grams per milliliter was detected by this multiphoton ionization configuration.
基金the National Natural Science Foundation of China under Grant No.19674017the National Climbing Project。
文摘A fully quantum nonperturbative method is developed to describe multiphoton ionization in intense fields. It is shown that, treating the radiation field with quantum electrodynamic(QED) theory enables u s to obtain the above-threshold ionization energy distribution spectrum in analytical form firstly. Moreover, in addition to the well-known semiclassical theory, the framework presented here, derived from a QED perspective, provides a new picture of the multiphoton 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 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.
文摘Late-stage modification of complex molecules via site-selective hydrodefluorination is a challenging endeavor.The selective activation of carbon-fluorine(C-F) bonds in the presence of multiple C-F bonds is of importance in organic synthesis and drug discovery.Herein,we describe the activation of C-F bonds via multiphoton photoredox catalysis to selectively produces a series of hydrodefluorinated compounds by simply tuning the reaction conditions.Moreover,this protocol was successfully applied to the late-stage functionalization of different drug-derivatives and the corresponding mono-,di-,and tri-defluorinated products were obtained in good to excellent yields.A detailed mechanistic investigation provides insight into the unprecedented hydrodefluorination pathway.
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the National Natural Science Foundation of China(52275294)the National Key Research and Development Program of China(2018YFA0703000).
文摘The designing and manufacturing of micro/nanoscale tools for delivery,diagnostic,and therapeutic are essential for their multiscale integration in the precision medicine field.Conventional three-dimensional(3D)printing approaches are not suitable for such kind of tools due to the accuracy limitation.Multiphoton polymerization(MPP)-based micro/nanomanufacturing is a noncontact,high-precision molding technology that has been widely used in the micro/nano field is a promising tool for micro/nanoscale related precision medicine.In this article the fundamentals of MPP-based technology and the required materials in precision medicine are overviewed.The biomedical applications in various scenarios are then summarized and categorized as delivery systems,microtissue modeling,surgery,and diagnosis.Finally,the existing challenges and future perspectives on MPP-based micro/nanomanufacturing for precision medicine are discussed,focusing on material design,process optimization,and practical applications to overcome its current limitations.
