To measure and control the electron motion in atoms and molecules by the strong laser field on the attosecond time scale is one of the research frontiers of atomic and molecular photophysics. It involves many new phen...To measure and control the electron motion in atoms and molecules by the strong laser field on the attosecond time scale is one of the research frontiers of atomic and molecular photophysics. It involves many new phenomena and processes and raises a series of questions of concepts, theories, and methods. Recent studies show that the Coulomb potential can cause the ionization time lag(about 100 attoseconds) between instants of the field maximum and the ionization-rate maximum. This lag can be understood as the response time of the electronic wave function to the strong-field-induced ionization event. It has a profound influence on the subsequent ultrafast dynamics of the ionized electron and can significantly change the time–frequency properties of electron trajectory(an important theoretical tool for attosecond measurement). Here, the research progress of response time and its implications on attosecond measurement are briefly introduced.展开更多
By numerically solving the time-dependent Schr¨odinger equation, we observe a remarkable strong-field interference pattern in the photoelectron momentum distribution of a hydrogen atom ionized by a few-cycles las...By numerically solving the time-dependent Schr¨odinger equation, we observe a remarkable strong-field interference pattern in the photoelectron momentum distribution of a hydrogen atom ionized by a few-cycles laser pulse. This interference pattern is joined together with the familiar near-forward strong-field photoelectron holographic interference. By applying the strong-field approximation theory, we investigate the formation of this interference pattern, which arises from the interference between the backward rescattered part and the direct part of the tunneling ionized electron wave packet. We demonstrate that this backward rescattered photoelectron holographic interference can also be observed in a more realistic parallel two-color laser field. These results pave a new way to look into the atomic and molecular structure with ultrafast timescale.展开更多
Coherent superposition of electronic states induces attosecond electron motion in molecules.We theoretically investigate the strong-field ionization of this superposition state by numerically solving the time-dependen...Coherent superposition of electronic states induces attosecond electron motion in molecules.We theoretically investigate the strong-field ionization of this superposition state by numerically solving the time-dependent Schrodinger equation.In the obtained photoelectron momentum distribution,an intriguing bifurcation structure appears in the strong-field holographic interference pattern.We demonstrate that this bifurcation structure directly provides complete information about the status of the transient wave function of the superposition state:the horizontal location of the bifurcation in the momentum distribution reveals the relative phase of the involved components of the superposition state and the vertical position indicates the relative coefficient.Thus,this bifurcation structure takes a snapshot of the transient electron wave packet of the superposition state and provides an intuitive way to monitor electron motion in molecules.展开更多
The Ammosov–Delone–Krainov(ADK) and Perelomov–Popov–Terent'ev(PPT) ionization models were widely used in strong-field physics and attosecond science due to their many attractive advantages such as simpler anal...The Ammosov–Delone–Krainov(ADK) and Perelomov–Popov–Terent'ev(PPT) ionization models were widely used in strong-field physics and attosecond science due to their many attractive advantages such as simpler analytical formula, less computational demands, and satisfied accuracy of ionization rate. Based on the density-functional theory, we systematically determine accurate structure parameters of 25 atoms, 24 positive ions and 13 negative ions and tabulate for future applications. The wave function with correct asymptotic behavior is obtained by solving the time-independent Schr?dinger equation with B-spline basis sets and the accurate structure parameters are extracted from this wave function in the asymptotic region. The accuracies of structure parameters are carefully examined by comparing the ionization probabilities(or yields) calculated by PPT and ADK models with those of solving the threedimensional time-dependent Schr?dinger equation and the experimental data.展开更多
Electronic processes within atoms and molecules reside on the timescale of attoseconds. Recent advances in the laserbased pump-probe interrogation techniques have made possible the temporal resolution of ultrafast ele...Electronic processes within atoms and molecules reside on the timescale of attoseconds. Recent advances in the laserbased pump-probe interrogation techniques have made possible the temporal resolution of ultrafast electronic processes on the attosecond timescale, including photoionization and tunneling ionization. These interrogation techniques include the attosecond streak camera, the reconstruction of attosecond beating by interference of two-photon transitions, and the attoclock. While the former two are usually employed to study photoionization processes, the latter is typically used to investigate tunneling ionization. In this review, we briefly overview these timing techniques towards an attosecond temporal resolution of ionization processes in atoms and molecules under intense laser fields. In particular, we review the backpropagation method, which is a novel hybrid quantum-classical approach towards the full characterization of tunneling ionization dynamics. Continued advances in the interrogation techniques promise to pave the pathway towards the exploration of ever faster dynamical processes on an ever shorter timescale.展开更多
Ionization of molecules in femtosecond laser fields is the most fundamental and important step of various strong-field physical processes. In this study, we experimentally investigate strong field ionization of linear...Ionization of molecules in femtosecond laser fields is the most fundamental and important step of various strong-field physical processes. In this study, we experimentally investigate strong field ionization of linear N_2O molecules using a time-of-flight mass spectrometer in 800-nm laser fields. Yields of the parent ion and different fragment ions are measured as a function of laser intensity in the range of 2.0×10^(13) W/cm^2 to 3.6×10^(14) W/cm^2. We also investigate the dependence of strong field ionization and dissociation of N_2O on laser ellipticity and polarization direction. The significant role of laser induced electron re-collision in the formation of highly charged fragment ions is proved. The physical mechanism of strong field ionization and fragmentation is discussed, based on our experimental results.展开更多
We develop the strong-field and higher-order expansion framework for the NUVO scalar geometry.Starting from the nonlinear field equation R_(g)=-c^(4)/8πGT obtained in a previous work,we perform systematic perturbativ...We develop the strong-field and higher-order expansion framework for the NUVO scalar geometry.Starting from the nonlinear field equation R_(g)=-c^(4)/8πGT obtained in a previous work,we perform systematic perturbative expansions of λ and the metric g_(μv)=λ^(2)η_(μv) to second and third order in the post-Newtonian hierarchy.The resulting expressions establish the analytic structure required to compute the post-Newtonian parameters(β,γ,δ,…)in the forthcoming flagship study.展开更多
Ultra-intense lasers can generate the strongest electromagnetic fields in laboratory conditions,and are expected to perform tests of quantum electrodynamics(QED)in yet unexplored parameter ranges.Such experiments requ...Ultra-intense lasers can generate the strongest electromagnetic fields in laboratory conditions,and are expected to perform tests of quantum electrodynamics(QED)in yet unexplored parameter ranges.Such experiments require knowledge of the field strengths and all possible interaction pathways.The latter can be simplified if a perfect,particlefree vacuum is present,thereby excluding competing interactions.We propose a method to evacuate all residual gas particles prior to QED interactions,based on tunnel ionization by a preceding auxiliary laser pulse and a static electric field.We present modelling and experimental results of testing this method on a 0.5 TW chirped pulse amplification laser system.Experimental results match well the simulations for the given conditions and thereby provide valuable understanding to extrapolate this method for QED experiments with PW-class laser systems where it can likewise be employed for in situ peak field strength characterization.展开更多
The spatial features of a light field, such as in the form of the optical singularities, provide a new degree of freedom for the application of light fields in different areas of science and technology. However, altho...The spatial features of a light field, such as in the form of the optical singularities, provide a new degree of freedom for the application of light fields in different areas of science and technology. However, although the exploration of structured light is growing rapidly, the investigation of strong-field photoionization using such light fields is noticeably lagging behind. Here, we present an experimental study that reveals the signatures of intense, structured light fields with controlled optical singularities in strong-field photoionization. The different types of optical singularities can be identified through photoionization observables,i.e., photoelectron momentum distributions(PMDs). By concurrently shifting the locations of the phase and polarization singularities, the focal electric field features can be designated, and subsequently, the photoionization appearances can be manipulated. In this process, the behaviors of the different intense optical singularities are clearly visualized by the PMDs. This work will advance both the strong-field science and singularity optics.展开更多
We present the generation of high-repetition-rate strong-field terahertz(THz)pulses from a thin 4-N,N-dimethylamino-4’-N’-methyl-stilbazolium 2,4,6-trimethylbenzenesulfonate(DSTMS)organic crystal pumped by an ytterb...We present the generation of high-repetition-rate strong-field terahertz(THz)pulses from a thin 4-N,N-dimethylamino-4’-N’-methyl-stilbazolium 2,4,6-trimethylbenzenesulfonate(DSTMS)organic crystal pumped by an ytterbium-doped yttrium aluminum garnet laser.The generated THz pulse energy reaches 932.8 nJ at 1 kHz repetition rate,with a conversion efficiency of 0.19%and a peak electric field of 819 kV/cm.At a repetition rate of 10 kHz,it is able to maintain a peak electric field of 236 kV/cm and an average THz power of 0.77 mW.The high-repetition-rate,strong-field THz source provides a convenient tool for the study of THz matter manipulation and THz spectroscopy.展开更多
Exploiting high-energy electron beams colliding into high-intensity laser pulses brings an opportunity to reach high values of the dimensionless rest-frame acceleration χ and thereby invoke processes described by str...Exploiting high-energy electron beams colliding into high-intensity laser pulses brings an opportunity to reach high values of the dimensionless rest-frame acceleration χ and thereby invoke processes described by strong-field quantum electrodynamics(SFQED).Measuring deviations from the results of Furry-picture perturbation theory in SFQED at high χ can be valuable for testing existing predictions,as well as for guiding further theoretical developments.Nevertheless,such experimental measurements are challenging due to the probabilistic nature of the interaction processes,dominating signals of low-χ interactions and limited capabilities to control and measure the alignment and synchronization in such collision experiments.Here we elaborate a methodology of using approximate Bayesian computations for drawing statistical inferences based on the results of many repeated experiments despite partially unknown collision parameters that vary between experiments.As a proof-of-principle,we consider the problem of inferring the effective mass change due to coupling with the strong-field environment.展开更多
Strong-field tunneling ionization is the first step for a broad class of phenomena in intense laser-atom/molecule interactions. Accurate information about the electron wave packet from strong-field tunneling ionizatio...Strong-field tunneling ionization is the first step for a broad class of phenomena in intense laser-atom/molecule interactions. Accurate information about the electron wave packet from strong-field tunneling ionization of atoms and molecules is of essential importance for understanding various tunneling ionization triggered processes. Here, we survey the property of the electron wave packet in tunneling ionization of molecules with a method based on strong-field photoelectron holography. By solving the time-dependent Schr ¨odinger equation, it is shown that the holographic interference in the photoelectron momentum distribution exhibits the asymmetric behavior with respect to the laser polarization direction, when the molecule is aligned with a nonzero angle to the linearly polarized laser field. We demonstrate that this asymmetry is due to the nonzero initial transverse displacement of the electron wave packet at tunneling. By analyzing the holographic interference, this transverse displacement for the launching of electron wave packet tunneling from the molecules is accurately retrieved. This displacement is directly related to the electron density distribution in molecules, and thus our work developed a novel concept for probing electronic structure in molecules.展开更多
基金Project supported by the National Natural Science Foundation of China(Grant No.91750111)the National Key Research and Development Program of China(Grant No.2018YFB0504400)。
文摘To measure and control the electron motion in atoms and molecules by the strong laser field on the attosecond time scale is one of the research frontiers of atomic and molecular photophysics. It involves many new phenomena and processes and raises a series of questions of concepts, theories, and methods. Recent studies show that the Coulomb potential can cause the ionization time lag(about 100 attoseconds) between instants of the field maximum and the ionization-rate maximum. This lag can be understood as the response time of the electronic wave function to the strong-field-induced ionization event. It has a profound influence on the subsequent ultrafast dynamics of the ionized electron and can significantly change the time–frequency properties of electron trajectory(an important theoretical tool for attosecond measurement). Here, the research progress of response time and its implications on attosecond measurement are briefly introduced.
基金Project supported by the Key Science and Technology Research of Henan Province,China(Grant Nos.162102210111 and 172102310471)the National Key Research and Development Program of China(Grant No.2017YFB0403502)
文摘By numerically solving the time-dependent Schr¨odinger equation, we observe a remarkable strong-field interference pattern in the photoelectron momentum distribution of a hydrogen atom ionized by a few-cycles laser pulse. This interference pattern is joined together with the familiar near-forward strong-field photoelectron holographic interference. By applying the strong-field approximation theory, we investigate the formation of this interference pattern, which arises from the interference between the backward rescattered part and the direct part of the tunneling ionized electron wave packet. We demonstrate that this backward rescattered photoelectron holographic interference can also be observed in a more realistic parallel two-color laser field. These results pave a new way to look into the atomic and molecular structure with ultrafast timescale.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11874163,11604108,and 11604388)the Program for HUST Academic Frontier Youth Teamthe Fundamental Research Funds for the Central Universities,China(HUST No.2017KFXKJC002)。
文摘Coherent superposition of electronic states induces attosecond electron motion in molecules.We theoretically investigate the strong-field ionization of this superposition state by numerically solving the time-dependent Schrodinger equation.In the obtained photoelectron momentum distribution,an intriguing bifurcation structure appears in the strong-field holographic interference pattern.We demonstrate that this bifurcation structure directly provides complete information about the status of the transient wave function of the superposition state:the horizontal location of the bifurcation in the momentum distribution reveals the relative phase of the involved components of the superposition state and the vertical position indicates the relative coefficient.Thus,this bifurcation structure takes a snapshot of the transient electron wave packet of the superposition state and provides an intuitive way to monitor electron motion in molecules.
基金Project supported by the National Natural Science Foundation of China under Grant Nos. 11664035, 11864037 and 11765018the Foundation of Northwest Normal University (No. NWNU-LKQN-17-1)。
文摘The Ammosov–Delone–Krainov(ADK) and Perelomov–Popov–Terent'ev(PPT) ionization models were widely used in strong-field physics and attosecond science due to their many attractive advantages such as simpler analytical formula, less computational demands, and satisfied accuracy of ionization rate. Based on the density-functional theory, we systematically determine accurate structure parameters of 25 atoms, 24 positive ions and 13 negative ions and tabulate for future applications. The wave function with correct asymptotic behavior is obtained by solving the time-independent Schr?dinger equation with B-spline basis sets and the accurate structure parameters are extracted from this wave function in the asymptotic region. The accuracies of structure parameters are carefully examined by comparing the ionization probabilities(or yields) calculated by PPT and ADK models with those of solving the threedimensional time-dependent Schr?dinger equation and the experimental data.
基金Project supported by the National Natural Science Foundation of China (Grant Nos.92150105,11834004,12227807,and 12241407)the Science and Technology Commission of Shanghai Municipality (Grant No.21ZR1420100)。
文摘Electronic processes within atoms and molecules reside on the timescale of attoseconds. Recent advances in the laserbased pump-probe interrogation techniques have made possible the temporal resolution of ultrafast electronic processes on the attosecond timescale, including photoionization and tunneling ionization. These interrogation techniques include the attosecond streak camera, the reconstruction of attosecond beating by interference of two-photon transitions, and the attoclock. While the former two are usually employed to study photoionization processes, the latter is typically used to investigate tunneling ionization. In this review, we briefly overview these timing techniques towards an attosecond temporal resolution of ionization processes in atoms and molecules under intense laser fields. In particular, we review the backpropagation method, which is a novel hybrid quantum-classical approach towards the full characterization of tunneling ionization dynamics. Continued advances in the interrogation techniques promise to pave the pathway towards the exploration of ever faster dynamical processes on an ever shorter timescale.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11534004,11874179,and 11704149)the Natural Science Foundation of Jilin Province,China(Grant No.20180101289JC)
文摘Ionization of molecules in femtosecond laser fields is the most fundamental and important step of various strong-field physical processes. In this study, we experimentally investigate strong field ionization of linear N_2O molecules using a time-of-flight mass spectrometer in 800-nm laser fields. Yields of the parent ion and different fragment ions are measured as a function of laser intensity in the range of 2.0×10^(13) W/cm^2 to 3.6×10^(14) W/cm^2. We also investigate the dependence of strong field ionization and dissociation of N_2O on laser ellipticity and polarization direction. The significant role of laser induced electron re-collision in the formation of highly charged fragment ions is proved. The physical mechanism of strong field ionization and fragmentation is discussed, based on our experimental results.
文摘We develop the strong-field and higher-order expansion framework for the NUVO scalar geometry.Starting from the nonlinear field equation R_(g)=-c^(4)/8πGT obtained in a previous work,we perform systematic perturbative expansions of λ and the metric g_(μv)=λ^(2)η_(μv) to second and third order in the post-Newtonian hierarchy.The resulting expressions establish the analytic structure required to compute the post-Newtonian parameters(β,γ,δ,…)in the forthcoming flagship study.
基金the China Scholarship Council for financial support during a visit of Qiqi Yu(File No.201908310159)to Helmholtz-Zentrum Dresden-Rossendorfthe National Natural Science Foundation of China(Grant No.11935008).
文摘Ultra-intense lasers can generate the strongest electromagnetic fields in laboratory conditions,and are expected to perform tests of quantum electrodynamics(QED)in yet unexplored parameter ranges.Such experiments require knowledge of the field strengths and all possible interaction pathways.The latter can be simplified if a perfect,particlefree vacuum is present,thereby excluding competing interactions.We propose a method to evacuate all residual gas particles prior to QED interactions,based on tunnel ionization by a preceding auxiliary laser pulse and a static electric field.We present modelling and experimental results of testing this method on a 0.5 TW chirped pulse amplification laser system.Experimental results match well the simulations for the given conditions and thereby provide valuable understanding to extrapolate this method for QED experiments with PW-class laser systems where it can likewise be employed for in situ peak field strength characterization.
基金supported by the National Natural Science Foundation of China (Grant Nos. 92050201, 11774013, and 11527901)。
文摘The spatial features of a light field, such as in the form of the optical singularities, provide a new degree of freedom for the application of light fields in different areas of science and technology. However, although the exploration of structured light is growing rapidly, the investigation of strong-field photoionization using such light fields is noticeably lagging behind. Here, we present an experimental study that reveals the signatures of intense, structured light fields with controlled optical singularities in strong-field photoionization. The different types of optical singularities can be identified through photoionization observables,i.e., photoelectron momentum distributions(PMDs). By concurrently shifting the locations of the phase and polarization singularities, the focal electric field features can be designated, and subsequently, the photoionization appearances can be manipulated. In this process, the behaviors of the different intense optical singularities are clearly visualized by the PMDs. This work will advance both the strong-field science and singularity optics.
基金supported by the National Key Research and Development Program of China(No.2022YFA1604401)the National Natural Science Foundation of China(Nos.12325409,62105346 and 12388102)+2 种基金the CAS Project for Young Scientists in Basic Research(No.YSBR-059)the Basic Research Project of the Shanghai Science and Technology Innovation Action Plan(No.20JC1416000)the Shanghai Pilot Program for Basic Research–Chinese Academy of Sciences,Shanghai Branch。
文摘We present the generation of high-repetition-rate strong-field terahertz(THz)pulses from a thin 4-N,N-dimethylamino-4’-N’-methyl-stilbazolium 2,4,6-trimethylbenzenesulfonate(DSTMS)organic crystal pumped by an ytterbium-doped yttrium aluminum garnet laser.The generated THz pulse energy reaches 932.8 nJ at 1 kHz repetition rate,with a conversion efficiency of 0.19%and a peak electric field of 819 kV/cm.At a repetition rate of 10 kHz,it is able to maintain a peak electric field of 236 kV/cm and an average THz power of 0.77 mW.The high-repetition-rate,strong-field THz source provides a convenient tool for the study of THz matter manipulation and THz spectroscopy.
基金support from the Swedish Research Council(Grant No.2017-05148 and No.201902376)provided by the National Academic Infrastructure for Supercomputing in Sweden(NAISS)at Tetralithpartially funded by the Swedish Research Council through grant agreement No.2022-06725
文摘Exploiting high-energy electron beams colliding into high-intensity laser pulses brings an opportunity to reach high values of the dimensionless rest-frame acceleration χ and thereby invoke processes described by strong-field quantum electrodynamics(SFQED).Measuring deviations from the results of Furry-picture perturbation theory in SFQED at high χ can be valuable for testing existing predictions,as well as for guiding further theoretical developments.Nevertheless,such experimental measurements are challenging due to the probabilistic nature of the interaction processes,dominating signals of low-χ interactions and limited capabilities to control and measure the alignment and synchronization in such collision experiments.Here we elaborate a methodology of using approximate Bayesian computations for drawing statistical inferences based on the results of many repeated experiments despite partially unknown collision parameters that vary between experiments.As a proof-of-principle,we consider the problem of inferring the effective mass change due to coupling with the strong-field environment.
基金supported by the National Key Research and Development Program of China (Grant No. 2019YFA0308300)the National Natural Science Foundation of China (Grant Nos. 11874163, 11934006, and12021004)。
文摘Strong-field tunneling ionization is the first step for a broad class of phenomena in intense laser-atom/molecule interactions. Accurate information about the electron wave packet from strong-field tunneling ionization of atoms and molecules is of essential importance for understanding various tunneling ionization triggered processes. Here, we survey the property of the electron wave packet in tunneling ionization of molecules with a method based on strong-field photoelectron holography. By solving the time-dependent Schr ¨odinger equation, it is shown that the holographic interference in the photoelectron momentum distribution exhibits the asymmetric behavior with respect to the laser polarization direction, when the molecule is aligned with a nonzero angle to the linearly polarized laser field. We demonstrate that this asymmetry is due to the nonzero initial transverse displacement of the electron wave packet at tunneling. By analyzing the holographic interference, this transverse displacement for the launching of electron wave packet tunneling from the molecules is accurately retrieved. This displacement is directly related to the electron density distribution in molecules, and thus our work developed a novel concept for probing electronic structure in molecules.
