Attosecond ionization time delays in strong-field physics

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 fo...     

强场非次序双电离中再碰撞动力学的强度依赖

利用三维经典系综模型系统地研究了不同强度线偏振激光脉冲驱动下He原子的非次序双电离.结果表明在非次序双电离中回碰电子的返回次数、两电子的碰撞距离和电子对的关联特性都强烈地依赖于激光强度.对于750 nm,随着激光强度的增加,单次返回诱导的非次序双电离事件逐渐减少,而多次返回事件的比例显著增加.对于1500 nm,随着激光强度的增加,前三次返回诱导的非次序双电离事件都会减少,返回次数大于3的轨道对非次序双电离的贡献逐渐增加.这是因为在高强度下每次返回过程中母核的库仑吸引对返回电子横向偏离的补偿较弱,所以需要更多次的返回来补偿电子的横向偏离以实现再碰撞.轨道分析表明非次序双电离中两电子的碰撞距离随激光波长和强度的增加而逐渐减小.最后讨论了非次序双电离中电子对的关联特性对返回次数的依赖.     

High-energy cutoff in the spectrum of strong-field nonsequential double ionization

Electron energy distributions of singly and doubly ionized helium in an intense 390 nm laser field have been measured at two intensities (0.8 PW/cm2 and 1.1 PW/cm2, where PW is defined as 10(15) W/cm2). Numerical solutions of the full-dimensional time-dependent helium Schr?dinger equation show excellent agreement with the experimental measurements. The high-energy portion of the two-electron energy distributions reveals an unexpected 5U(p) cutoff for the double ionization (DI) process and leads to a proposed model for DI below the quasiclassical threshold.     

Probing time delay of strong-field resonant above-threshold ionization

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.     

Observation of a transition in the dynamics of strong-field double ionization

The double ionization of argon and xenon in an intense laser field has been studied in detail using an electron-ion coincidence technique. The observed double ionization electron spectra in xenon show resonancelike structures here resolved for the first time. In argon, the featureless spectra are consistent with rescattering. This represents a clear transition in the dynamics of strong-field double ionization, analogous to the well-known transition between the tunneling and multiphoton regimes in single ionization.     

Classical effects of laser pulse duration on strong-field double ionization

We use classical electron ensembles and the aligned-electron approximation to examine the effect of laser pulse duration on the dynamics of strong-field double ionization. We cover the range of intensities 10(14)-10(16) W/cm2 for the laser wavelength 780 nm. The classical scenario suggests that the highest rate of recollision occurs early in the pulse and promotes double-ionization production in few-cycle pulses. In addition, the purely classical ensemble calculation predicts an exponentially decreasing recollision rate with each subsequent half cycle. We confirm the exponential behavior by trajectory back analysis.     

强激光场中原子双电离动力学复杂机制分析

通过数值求解薛定谔方程并用“抓拍”(snapshot)的方式观测两电子动量分布,我们研究了超强超快激光场中原子发生非次序双电离的不同机制。我们的模拟表明“抓拍”过程中双电离波函数的选取范围对两电子动量分布图样的特征和分布范围等都有显著的影响。图样中这种由于不同的观测范围导致的明显区别直接地影响我们对非次序双电离动力学过程的分辨。为此本文即结合经典再散射三步模型,详细分析了“抓拍”过程中双电离波函数范围的选取,并深入讨论了不同的非次序双电离机制及其对应的动量分布的特征。本文的结果将给相关的实验研究提供有益的参考。     

Transition from strong-field sequential to nonsequential double ionization at near-infrared wavelengths and low intensities

Within a quantum-mechanical model, we investigate strong-field double ionization of a model helium atom by near-infrared, linearly polarized laser pulses at intensities far below the recollision threshold. The quantum simulations show a clear mechanism change from sequential to nonsequential double ionization (NSDI) as the laser intensity increases. For NSDI, the two-electron correlated momentum distribution exhibits a strong final-state Coulomb repulsion effect for high-energy photoelectrons, but absent for low-energy photoelectrons. This repulsion effect is ascribed to field double ionization from doubly-excited states populated by recollision of the first ionized electron when it returns to the parent ion. Such recollision-induced excited states are absent at ultraviolet wavelengths due to the very low returning kinetic energies, resulting to the absence of final-state repulsion effect in NSDI.     

Correlated two-electron momentum spectra for strong-field nonsequential double ionization of He at 800 nm

We report on a kinematically complete experiment on nonsequential double ionization of He by 25 fs 800 nm laser pulses at 1.5 PW/cm;{2}. The suppression of the recollision-induced excitation at this high intensity allows us to address in a clean way direct (e,2e) ionization by the recolliding electron. In contrast with earlier experimental results, but in agreement with various theoretical predictions, the two-electron momentum distributions along the laser polarization axis exhibit a pronounced V-shaped structure, which can be explained by the role of Coulomb repulsion and typical (e,2e) kinematics.     

Dynamics of strong-field double ionization of H_2 in co-rotating two-color circularly polarized laser fields

Double ionization of H_2 in a co-rotating two-color circularly polarized(TCCP) laser field is theoretically investigated. By changing the ratio of electric field peak amplitudes of the TCCP laser pulses, the double ionization probability as a function of the laser intensity shows a clear knee structure, which is suppressed significantly in the case of the atom. Due to the large spatial range of the electronic initial distribution, with the analysis of classical trajectories of ionized electrons, it is found that the ionization of the electron in the farther distance increases the probability of recollision. Furthermore, the yield of nonsequential double ionization created by the recollision can be enhanced by controlling the amplitude ratio of the TCCP laser field.     

Backward rescattered photoelectron holography in strong-field ionization

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.     

Low-frequency strong-field ionization and excitation of hydrogen atom

The dynamics of hydrogen atom in the presence of a strong radiation field of the titanium-sapphire laser is studied for the Keldysh parameters γ ≥ 1 and γ ≤ 1. It is demonstrated that the ionization is supplemented with the effective population of the excited states with the principal quantum numbers n = 5–10 in the entire range of variation in the Keldysh parameter. The population of the excited Rydberg states can be interpreted as a consequence of the multiphoton resonance involving the initial 1s state and a group of excited states in the vicinity of the continuum boundary with the simultaneous repopulation of these states by Λ-type Raman transitions under the action of the laser field. The resulting coherent Rydberg packet appears to be stable with respect to ionization, so that the ionization of the atomic system in the presence of strong electromagnetic field is suppressed. Physical reasons for the stabilization are discussed. An interpretation of the effective population of the Rydberg states in the recent experiments on the ionization of atomic helium by the titanium-sapphire laser is proposed.     

Effects of double pulses in strong-field photoionization

The dynamics of the bound state population and the photoelectron energy spectra due to photoionization by a double pulse are calculated for a model atomic system. The splitting of the ATI peaks due to the structure of the pulse is presented and discussed.     

Limits on tunneling theories of strong-field ionization

It is shown that tunneling theories of ionization by lasers are subject to upper and lower bounds on the Keldysh parameter gamma. The tunneling limit, gamma-->0, applies to ionization by quasistatic electric fields, but not by laser fields. For lasers, the gamma-->0 limit requires a relativistic treatment. Bounds on the applicability of tunneling theories depend on parameters other than gamma, confirming the rule that strong-field phenomena require more than one dimensionless parameter for scaling.     

Angular momentum distribution in strong-field frustrated tunneling ionization

Using the classical-trajectory Monte Carlo model, we have theoretically studied the angular momentum distribution of frustrated tunneling ionization(FTI) of atoms in strong laser fields. Our results show that the angular momentum distribution of the FTI events exhibits a double-hump structure. With this classical model, we back traced the tunneling coordinates, i.e., the tunneling time and initial transverse momentum at tunneling ionization. It is shown that for the events tunneling ionized at the rising edge of the electric field,the final angular momentum exhibits a strong dependence on the initial transverse momentum at tunneling.While for the events ionized at the falling edge, there is a relatively harder recollision between the returning electron and the parent ion, leading to the angular momentum losing the correlation with the initial transverse momentum. Our study suggests that the angular momentum of the FTI events could be manipulated by controlling the initial coordinates of the tunneling ionization.     

Determination of structure parameters in strong-field ionization models of atoms

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 Schrödinger 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 three-dimensional time-dependent Schrödinger equation and the experimental data.     

Exploration of strong-field double ionization of C_3H_6 with the structures of propene and cyclopropane in intense laser fields

By using classical ensemble method, we investigate the double ionization of C_3H_6 molecule with different structures(propene and cyclopropane) in intense laser fields. The numerical results show that the non-sequential double ionization occurs in propene molecule rather than cyclopropane molecule in 1200 nm laser field. To further explain this interesting phenomenon, the momentum distribution of double ionized electrons is presented and the result presents the finger-like structure at about 30 TW/cm~2 of propene molecule, and this structure is more obvious than that in cyclopropane molecule.The above phenomena are also demonstrated by analysing the energy distributions of double-ionized electrons versus time. Moreover, we also investigated the angular distribution at the end of pulse, which is different between propene and cyclopropane.     

Dynamic polarization in the strong-field ionization of small metal clusters

We report on the strong field ionization of small transition metal clusters (nickel, Ni(n) n=1-36) within the quasistatic regime at an infrared wavelength of 1.5 microm and at intensities up to 2 x 10(14) W/cm(2). From ion yields in a constant axial intensity beam, we obtained saturation intensities for the individual Ni(n) clusters. As compared to quasistatic, single active electron calculations, a dramatic suppression of ionization was observed. Dynamic polarization in the laser field likely leads to strong multielectron screening of the "active" electron. Representing the metal clusters as classical conducting spheres, we obtained, via a barrier suppression calculation, the classical ionization rates. Agreement was obtained for larger clusters with n>10 when the dynamic polarization was taken into account, emphasizing the multielectron nature of the ionization suppression.     

Simulation of above-threshold ionization experiments using the strong-field approximation

Recently performed above-threshold ionization (ATI) experiments with noble gases allow the determination of the complete energy and angular distribution of the emitted photoelectrons. In order to simulate such experiments, we have generalized our numerical code for the calculation of ATI spectra in order to achieve a realistic simulation of ATI of the noble gases He, Ne, Ar, Kr, and Xe. Our method is based on an improved version of the strong-field approximation and includes focal averaging. A semiclassical analysis of the dependence of the cutoff law on the photoelectron emission angle is presented. The effects of channel closings on the high-energy spectra are analyzed.