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Physical Review A

Steering continuum electron dynamics by low-energy attosecond streaking

Ji-Wei Geng, Wei-Hao Xiong, Xiang-Ru Xiao, Qihuang Gong, Liang-You Peng

Published Aug 15, 2016• 3 citations
Publisher

Abstract

A semiclassical model is developed to understand the electronic dynamics in the low-energy attosecond streaking. Under a relatively strong infrared (IR) pulse, the low-energy part of photoelectrons initialized by a single attosecond pulse (SAP) can either rescatter with the ionic core and induce interferences structures in the momentum spectra of the ionized electrons or be recaptured into the Rydberg states. The Coulomb potential plays essential roles in both the electron rescattering and recapturing processes. We find that by changing the time delay between the SAP and the IR pulse, the photoelectrons yield or the population of the Rydberg states can be effectively controlled. The present study demonstrates a fascinating way to steer the electron motion in the continuum.

DOI
10.1103/physreva.94.023411

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A semiclassical model is developed to understand the electronic dynamics in the low-energy attosecond streaking. Under a relatively strong infrared (IR) pulse, the low-energy part of photoelectrons initialized by a single attosecond pulse (SAP) can either rescatter with the ionic core and induce interferences structures in the momentum spectra of the ionized electrons or be recaptured into the Rydberg states. The Coulomb potential plays essential roles in both the electron rescattering and recapturing processes. We find that by changing the time delay between the SAP and the IR pulse, the photoelectrons yield or the population of the Rydberg states can be effectively controlled. The present study demonstrates a fascinating way to steer the electron motion in the continuum.
By the numerical solution to the time-dependent Schr\"odinger equation, we observe a remarkable asymmetry in the photoelectron streaking spectra when the He+{\mathrm{He}}^{+}He+ ion is ionized by an attosecond pulse from the 2s2s2s state in the presence of a weak infrared pulse. An analytical theory based on the modified perturbation theory is developed to quantitatively account for the underlying mechanism. We find that a transition occurs between the degenerate 2s2s2s and 2p2p2p states under the influence of the infrared electric field before the arrival of the attosecond pulse. The observed asymmetry in the attosecond streaking is formed by the interference of photoelectrons ionized from the 2s2s2s and 2p2p2p states. Using the sensitivity of the asymmetry to the infrared (IR) electric field at the moment of attosecond photoionization, we show that the present finding provides a highly reliable way to fully characterize the IR waveform in the streaking experiment.
We study the two-dimensional photoelectron momentum distribution in a synthesized field of an attosecond pulse and a weak infrared femtosecond pulse by solving the time-dependent Schr\"odinger equation of He atoms. The photoelectron momentum spectra reveal fruitful interference structures. With a semiclassical model, we show that some of the photoelectron interference structures come from the interference between the direct and backward-scattering electron trajectories. Those backward-scattering electrons are freed by the attosecond pulse and then are hard rescattered with parent ions by the streaking infrared field. By changing the phase delay between the attosecond pulse and the infrared laser field, we find that two kinds of backward-scattering electron trajectories will contribute to the holographic pattern. We show that backward-scattering holography can be explored with attosecond streaking experiments.
Attosecond time-resolved electron tunneling dynamics have been investigated by using attosecond angular streaking spectroscopy, where a clock reference to the laser field vector is required in atomic strong-field ionization and the situation becomes complicated in molecules. Here we reveal a resonant ionization process via a transient state by developing an electron-tunneling-site-resolved molecular attoclock in Ar-Kr^{+}. Two distinct deflection angles are observed in the photoelectron angular distribution in the molecular frame, corresponding to the direct and resonant ionization pathways. We find the electron is temporally trapped in the Coulomb potential wells of the Ar-Kr^{+} before finally releasing into the continuum when the electron tunnels through the internal barrier. By utilizing the direct tunneling ionization as a self-referenced arm of the attoclock, the time delay of the electron trapped in the resonant state is revealed to be 3.50±0.04 fs. Our results give an impetus to exploring the ultrafast electron dynamics in complex systems and also endow a semiclassical presentation of the electron trapping dynamics in a quantum resonant state.
The past thirty years witnessed rapid developing of strong field physics that leads to the first generation of attosecond (10−18 s) pulses. The duration of available pulses has recently been reduced to less than 100 as, approaching the Kepler period of a classical electron revolving around the nucleus. For the first time, electron motions inside atoms, molecules and solids can be traced, probed and even steered in real time. It pushed the study on ultrafast dynamic processes into a new frontier, giving birth to attosecond physics. The development of attosecond pulses provides unprecedented coherent ultrashort XUV (extreme ultra-violet) of soft X-ray sources that enable imaging the atomic structure and resolving the related quantum dynamics for matter science. In particular, it allows the probing and monitoring of electron dynamics in the natural time scale of attoseconds with atomic spatial resolution. The generation and applications of attosecond pulses are directly related to the control and manipulation of the sub-cycle electron dynamics. Recent studies on the correlated multielectron dynamics have provided insight into the optical and dynamical properties of matter in the perspectives of time, phase and entanglement. It deepens our understanding on some of the fundamental questions, e.g., how the single or multiple photons are absorbed and how short are the quantum processes such as photoionization, tunneling ionization and charge migration. Although currently attosecond pulses are limited by the flux and pulse duration, the combination of attosecond pulses with intense infrared laser pulses paves new ways of controlling and probing electron dynamics in the domains of energy, time and space that lays the foundation for petahertz optoelectronics and attosecond pulse based transient spectroscopy. In this review, we will first briefly summarize the advancement of strong field and ultrafast physics including the relevant experimental findings, the theoretical explorations, the related technologies and the possible applications. Then we focus on the sub-cycle electron or multielectron dynamics and their manifestation on the ionization and coherent radiation properties. We start with the time behavior of Fano resonance and how it can be probed in time domain. In section 2, the correlated electron dynamics is discussed in term of anti-screening effect and Pauli effect that influence strong field ionization and high harmonic generation processes. In section 3, the coherent emission with frequency from terahertz to soft XUV and their joint measurement are discussed by emphasizing the generation mechanism of terahertz wave in two-color laser pulses. The developed high-harmonic and terahertz wave spectroscopy (HATS) is shown capable of imaging the molecular structure and dynamics. In section 4, the time-resolving of electron and hole dynamics and their coherence is proposed based on attosecond transient absorption technique. The coherence of ionization and the correlated electron dynamics is hinted crucial for electron-hole interaction. The topics are very limited and mainly selected from the perspectives of our group.
We theoretically study the infrared (IR)-dressed photoionization of atoms excited by extreme ultraviolet attosecond pulse trains above ionization threshold. The initial state of atoms is treated perturbatively by the IR field, and the continuum states are considered as Coulomb–Volkov (CV) waves. CV waves can much reduce the gauge difference calculated with Volkov waves, and, in general, the contribution of ground-state perturbation to the photoelectron spectrum is negligible. Our calculations show qualitative agreement with the experimental results [Phys. Rev. Lett. 95, 013001 (2005)]. An evident dependence of the photoelectron spectrum on the delay phase between the IR field and the attosecond pulse train is exhibited in both helium and argon. The angular distribution of photoelectrons with various IR polarizations and the corresponding photoelectron spectra are presented. The linearly polarized IR fields are shown to have a higher controlling capability of the spectrum via IR delay phases than the circularly polarized fields. On the other hand, the circularly polarized IR fields have a fruitful angular dependence of photoelectrons with various IR delay phases.
Laser-induced electron tunneling ionization from atoms and molecules plays as the trigger for a broad class of interesting strong-field phenomena in attosecond community. Understanding the time of electron tunneling ionization is vital to achieving the ultimate accuracy in attosecond metrology. We propose a novel attosecond photoelectron interferometer, which is based on the interference of the direct and near-forward rescattering electron wave packets, to determine the time information characterizing the tunneling process. Adding a weak perturbation in orthogonal to the strong fundamental field, the phases of the direct and the near-forward rescattering electron wave packets are modified, leading to the shift of the interferogram in the photoelectron momentum distributions. By analyzing the response of the interferogram to the perturbation, the real part of the ionization time, which denotes the instant when the electron exits the potential barrier, and the associated rescattering time are precisely retrieved. Moreover, the imaginary part of the ionization time, which has been interpreted as a quantity related to electron motion under the potential barrier, is also unambiguously determined.