Coherent electron scattering captured by an attosecond quantum stroboscope

We demonstrate a quantum stroboscope based on a sequence of identical attosecond pulses that are used to release electrons into a strong infrared (IR) laser field exactly once per laser cycle. The resulting electron momentum distributions are recorded as a function of time delay between the IR laser and the attosecond pulse train using a velocity map imaging spectrometer. Because our train of attosecond pulses creates a train of identical electron wave packets, a single ionization event can be studied stroboscopically. This technique has enabled us to image the coherent electron scattering that takes place when the IR field is sufficiently strong to reverse the initial direction of the electron motion causing it to rescatter from its parent ion.     

Attosecond control of ionization by wave-packet interference

A train of attosecond pulses, synchronized to an infrared (IR) laser field, is used to create a series of electron wave packets (EWPs) that are below the ionization threshold in .helium. The ionization probability is found to strongly oscillate with the delay between the IR and attosecond fields twice per IR laser cycle. Calculations that reproduce the experimental results demonstrate that this ionization control results from interference between transiently bound EWPs created by different pulses in the train. In this way, we are able to observe, for the first time, attosecond wave-packet interference in a strongly driven atomic system.     

Optical detection of attosecond ionization induced by a few-cycle laser field in a transparent dielectric material

We observe an optical signature induced by the modulation of electron density inside a bulk transparent solid that is quasiperiodically ionized on an attosecond time scale by electric field peaks of a focused few-cycle laser pulse. The emitted optical signal resulting from the attosecond ionization dynamics is spatially, temporally and spectrally isolated from concomitant optical responses through the use of a noncollinear pump-probe technique. The method holds promise for developing an attosecond metrology for bulk solids, in which, unlike in the established attosecond metrology of gases and surfaces, direct detection of charged particles is unfeasible.     

Attosecond angle-resolved photoelectron spectroscopy

We report experiments on the characterization of a train of attosecond pulses obtained by high-harmonic generation, using mixed-color (XUV+IR) atomic two-photon ionization and electron detection on a velocity map imaging detector. We demonstrate that the relative phase of the harmonics is encoded both in the photoelectron yield and the angular distribution as a function of XUV-IR time delay, thus making the technique suitable for the detection of single attosecond pulses. The timing of the attosecond pulse with respect to the field oscillation of the driving laser critically depends on the target gas used to generate the harmonics.     

Direct XUV probing of attosecond electron recollision

We demonstrate that the recolliding electron wave packet, fundamental to many strong field phenomena, can be directly imaged with sub-A spatial and attosecond temporal resolution using attosecond extreme ultraviolet (XUV) pulses. When the recolliding electron revisits the parent ion, it can absorb an XUV photon yielding high energy electron and thereby providing a measurement of the electron energy at the moment of recollision. The full temporal evolution of the recollision wave packet can be reconstructed by measuring the photoelectron spectra for different time delays between the driving laser and the attosecond XUV probe. The strength of the photoelectron signal can be used to characterize the spatial distribution of the electron density in the longitudinal direction. Elliptical polarization can be used to characterize the electron probability in transversal direction.     

Attosecond streaking of correlated two-electron transitions in helium

We present fully ab initio simulations of attosecond streaking for ionization of helium accompanied by shakeup of the second electron. This process represents a prototypical case for strongly correlated electron dynamics on the attosecond time scale. We show that streaking spectroscopy can provide detailed information on the Eisenbud-Wigner-Smith time delay as well as on the infrared-field dressing of both bound and continuum states. We find a novel contribution to the streaking delay that stems from the interplay of electron-electron and infrared-field interactions in the exit channel. We quantify all the contributions with attosecond precision and provide a benchmark for future experiments.     

Attosecond control in photoionization of hydrogen molecules

We report experiments where hydrogen molecules were dissociatively ionized by an attosecond pulse train in the presence of a near-infrared field. Fragment ion yields from distinguishable ionization channels oscillate with a period that is half the optical cycle of the IR field. For molecules aligned parallel to the laser polarization axis, the oscillations are reproduced in two-electron quantum simulations, and can be explained in terms of an interference between ionization pathways that involve different harmonic orders and a laser-induced coupling between the 1sσ(g) and 2pσ(u) states of the molecular ion. This leads to a situation where the ionization probability is sensitive to the instantaneous polarization of the molecule by the IR electric field and demonstrates that we have probed the IR-induced electron dynamics with attosecond pulses.     

Internal momentum state mapping using high harmonic radiation

We numerically demonstrate so-far undescribed features in ionization and high harmonic generation from bound states with nonvanishing electronic angular momentum. The states' modified response to a strong laser pulse can be exploited for novel measurement and pulse production schemes. It is shown that angularly asymmetric tunneling from the states can be mapped onto variations of high harmonic intensities and that near-circularly polarized isolated attosecond extreme ultraviolet or x-ray pulses can be produced.     

Multiple ionization bursts in laser-driven hydrogen molecular ion

Theoretical study on H2(+) in an intense infrared laser field on the attosecond time scale reveals that the molecular ion shows multiple bursts of ionization within a half-cycle of the laser field oscillation, in contrast to the widely accepted tunnel ionization picture for an atom. These bursts are found to be induced by transient localization of the electron at one of the nuclei, and a relation between the time instants of the localization and the vector potential of the laser light is derived. A scheme is proposed to probe the localization dynamics by an extreme ultraviolet laser pulse.     

Ionization of atoms by chirped attosecond pulses

We investigate the ionization dynamics of atoms by chirped attosecond pulses using the strong field approximation method. The pulse parameters are carefully chosen in the regime where the strong field approximation method is valid. We analyse the effects of the chirp of attosecond pulses on the energy distributions and the corresponding left-right asymmetry of the ionized electrons. For a single chirped attosecond pulse, the ionized electrons can be redistributed and the left-right asymmetry shows oscillations because of the introduction of the chirp. For time-delayed double attosecond pulses at different intensities with the weaker one chirped, exchanging the order of the two pulses shows a relative shift of the energy spectra, which can be explained by the different effective time delays of different frequency components because of the chirp.     

Amplitude and phase reconstruction of electron wave packets for probing ultrafast photoionization dynamics

Ultrafast atomic processes, such as excitation and ionization occurring on the femtosecond or shorter time scale, were explored by employing attosecond high-harmonic pulses. With the absorption of a suitable high-harmonic photon a He atom was ionized, or resonantly excited with further ionization by absorbing a number of infrared photons. The electron wave packets liberated by the two processes generated an interference containing the information on ultrafast atomic dynamics. The attosecond electron wave packet, including the phase, from the ground state was reconstructed first and, subsequently, that from the 1s3p state was retrieved by applying the holographic technique to the photoelectron spectra comprising the interference between the two ionization paths. The reconstructed electron wave packet revealed details of the ultrafast photoionization dynamics, such as the instantaneous two-photon ionization rate.     

Single attosecond burst generation during ionization of excited atoms by intense ultrashort laser pulses

We develop an analytical approach to describing the generation of a single attosecond burst during barrier-suppression ionization of a hydrogen atom by an intense laser pulse. We derive analytical expressions that describe the evolution of the electron wave packet in the time interval between the detachment from the atom and the collision with the parent ion for an arbitrary initial atomic state by assuming the atom to be fully ionized in one laser-field half-period. For various s-states, we derive expressions for the profile of the attosecond burst generated when the electron packet collides with the ion and analyze the dependence of its generation efficiency on the principal quantum number n of the initial atomic state. The results obtained are compared with the results of three-dimensional numerical calculations. We show that the attosecond pulse generation efficiency can be several orders of magnitude higher than that in the case of ionization from the ground state when pre-excited atomic states are used.     

Control mechanism of atomic ionization and high-order harmonic generation assisted by attosecond pulses

Attosecond pulses combined with infrared laser constitute a powerful tool for controlling atomic photoionization and high-order harmonic generation (HHG). We apply the intense-field many-body S-matrix theory to solve such two-pulse excitation problems. The theory can give a clear explanation for the oscillation of ionization probability as a function of time delay between infrared field and attosecond pulses with central frequency lying below ionization threshold at moderate infrared intensities. The HHG assisted by such attosecond pulses is also interpreted. In addition to a known dramatic enhancement of HHG, a harmonic emission from rapid oscillation of bound-state population caused by the counter-rotating wave is presented.     

Electron dynamics triggered by double attosecond pulses: Simulations based on time-dependent density functional theory

In order to observe the high-field effect, the external laser field must reach its peak intensity before the electron ionization. To this end, it is important to reduce pulse duration to typical attosecond timescale. In this paper, the interaction electron dynamics between attosecond pulses and dielectric is investigated within the time-dependent density functional theory. Taking the CaF₂ crystal as an example, we give a comparison of electron dynamics response between single and double pulses. Moreover, the nonlinear energy absorption and electron excitation processes are simulated by adjusting the polarization direction of the sub-pulse. Present results demonstrate that the double pulses show lower electron excitation and energy absorption than the single pulse, which is in accordance with experimental higher ablation threshold and smaller heat-affected zones of the double pulses. In addition, the curves of final excited electron number and energy absorption exhibit the quasi-symmetry about the axis of 180°, which has not been reported yet.     

Attosecond electron wave packet dynamics in strong laser fields

We use a train of sub-200 attosecond extreme ultraviolet (XUV) pulses with energies just above the ionization threshold in argon to create a train of temporally localized electron wave packets. We study the energy transfer from a strong infrared (IR) laser field to the ionized electrons as a function of the delay between the XUV and IR fields. When the wave packets are born at the zero crossings of the IR field, a significant amount of energy (approximately 20 eV) is transferred from the field to the electrons. This results in dramatically enhanced above-threshold ionization in conditions where the IR field alone does not induce any significant ionization. Because both the energy and duration of the wave packets can be varied independently of the IR laser, they are valuable tools for studying and controlling strong-field processes.     

Frequency-resolved optical gating of isolated attosecond pulses in the extreme ultraviolet

The pulse shape and phase of isolated attosecond extreme ultraviolet (XUV) pulses with a duration of 860 asec have been determined simultaneously by using frequency-resolved optical gating based on two-photon above-threshold ionization with 28-eV photons in He. From the detailed characterization, we succeeded in shaping isolated XUV pulses on an attosecond time scale by precise dispersion control with Ar gas density or by changing the driving pulse width. These results offer a novel way to excite and observe an electron motion in atoms and molecules.     

空间非均匀啁啾双色场驱动下氦离子的高次谐波以及孤立阿秒脉冲的产生

本文理论上研究了初态为基态与第一激发态等权叠加的一维氦离子在空间非均匀啁啾双色场驱动下氦离子的高次谐波发射及孤立阿秒脉冲的产生. 研究表明, 一维氦离子在空间非均匀啁啾双色场驱动下发射的高次谐波相对于均匀场情况截止位置得到明显扩展, 得到了光滑的超连续谱,并应用半经典三步模型解释了高次谐波发射的物理机理. 通过小波变换的方法对连续谱进行了时频分析, 并且与电子的经典运动轨迹进行了对比分析, 结果显示在空间非均匀场中长量子轨道消失, 短量子轨道加强. 讨论了空间非均匀啁啾双色场中时间延迟对谐波和孤立阿秒脉冲产生的影响, 发现适当调整时间延迟值可以得到较大延展的光滑的超连续谐波谱, 本方案中时间延迟为t₀=1.6πup/ω₁时得到了最大延展, 通过对谐波中600次到680次(80次)谐波合成得到32 as的孤立脉冲.     

Investigation of vortex arms in electron vortices by counter-rotating elliptically polarized attosecond laser pulses

We theoretically investigate the vortex patterns in photoelectron momentum distributions of He⁺driven by counter-rotating elliptically polarized,time delayed attosecond laser pulses by numerically solving the two-dimensional time-dependent Schrodinger equation.It is found that the number of vortex arms is extremely sensitive to the ellipticity and wavelength of counterrotating elliptically polarized laser pulses,which is illustrated by the attosecond perturbation ionization models.In addition,the effect of different time delays between two pulses on the interference patterns is also investigated and the corresponding physical mechanism is demonstrated.Since the wavelength,ellipticity and time delay have a significant effect on the vortex interference patterns,this may be a new method for laser field detection.     

Attosecond burst and high-harmonic generation in molecular ionization by ultrashort laser pulses

It is shown that the efficiency of attosecond pulse and high-harmonic generation in the ionization of excited molecular structures by a powerful femtosecond optical pulse can appreciably exceed the efficiency of analogous processes in atomic systems. This is due to the presence of a delocalized electron wave-packet component in the nonequilibrium molecular states, resulting in an increase of the number of particles that are effectively involved in the bremsstrahlung generation in the course of recollisions of laser-accelerated electrons with molecular core. Calculations suggest that, by optimizing the nonlinear response of molecular systems in the ionization process, one can develop compact sources of coherent vacuum ultraviolet and X-ray radiation with luminance at a level that is presently achieved only at large-scale accelerator facilities with free-electron lasers.