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Physical Review A

Direct visualization of the transverse photoemission position within molecules via strong-field photoelectron holography

Jia Min Tan, Qinghua Ke, Dian Wang, Xiang Hao, Jialing Xie, Yu Guo, Xue Xu, Quanying Wu

Published Aug 7, 2023• 4 citations
Publisher

Abstract

Laser-induced tunneling ionization triggers a broad class of strong-field phenomena in the attosecond community. The understanding and application of these ultrafast phenomena require accurate knowledge of the position information for the tunneling electron wave packet (EWP). Here, with strong-field photoelectron holography, we theoretically demonstrate a scheme to retrieve the position of the EWP emitted from molecules in the direction perpendicular to the tunnel. In our scheme, the photoelectron momentum distributions from strong-field tunneling ionization are obtained by solving the time-dependent Schr\"odinger equation. When the molecule is aligned with a nonzero angle to the linearly polarized laser field, a distinct shift of the holographic pattern in the photoelectron momentum distribution is observed. With the quantum-orbit model, we demonstrate that the shift of the holographic pattern is caused by a nonzero initial transverse position of the EWP immediately after tunneling. By tracing their exact correspondence and examining the shift of the holographic pattern, the transverse emission position of the tunnel-ionized EWP is probed accurately. Furthermore, we demonstrate that the complex Coulomb interaction can be safely canceled in our scheme by performing the scheme for both of the model molecules with the short-range and Coulomb potentials. The validity and accuracy of our scheme are confirmed by its application to different molecules, alignments, and laser parameters.

DOI
10.1103/physreva.108.023110

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Laser-induced tunneling ionization triggers a broad class of strong-field phenomena in the attosecond community. The understanding and application of these ultrafast phenomena require accurate knowledge of the position information for the tunneling electron wave packet (EWP). Here, with strong-field photoelectron holography, we theoretically demonstrate a scheme to retrieve the position of the EWP emitted from molecules in the direction perpendicular to the tunnel. In our scheme, the photoelectron momentum distributions from strong-field tunneling ionization are obtained by solving the time-dependent Schr"odinger equation. When the molecule is aligned with a nonzero angle to the linearly polarized laser field, a distinct shift of the holographic pattern in the photoelectron momentum distribution is observed. With the quantum-orbit model, we demonstrate that the shift of the holographic pattern is caused by a nonzero initial transverse position of the EWP immediately after tunneling. By tracing their exact correspondence and examining the shift of the holographic pattern, the transverse emission position of the tunnel-ionized EWP is probed accurately. Furthermore, we demonstrate that the complex Coulomb interaction can be safely canceled in our scheme by performing the scheme for both of the model molecules with the short-range and Coulomb potentials. The validity and accuracy of our scheme are confirmed by its application to different molecules, alignments, and laser parameters.
Laser-induced electron tunneling underlies numerous emerging spectroscopic techniques to probe attosecond electron dynamics in atoms and molecules. The improvement of those techniques requires an accurate knowledge of the exit momentum for the tunneling wave packet. Here we demonstrate a photoelectron interferometric scheme to probe the electron momentum longitudinal to the tunnel direction at the tunnel exit by measuring the photoelectron holographic pattern in an orthogonally polarized two-color laser pulse. In this scheme, we use a perturbative 400-nm laser field to modulate the photoelectron holographic fringes generated by a strong 800-nm pulse. The fringe shift offers direct experimental access to the intermediate canonical momentum of the rescattering electron, allowing us to reconstruct the momentum offset at the tunnel exit with high accuracy. Our result unambiguously proves the existence of nonzero initial longitudinal momentum at the tunnel exit and provides fundamental insights into the nonquasistatic nature of the strong-field tunneling.
Strong-field tunneling ionization is the initial step for various ultrafast dynamics in intense laser-atom and/or molecule interactions. Time-resolving tunneling ionization is of crucial importance for accurately understanding these ultrafast processes. In our previous work [Phys. Rev. Lett. 121, 253203 (2018).], we proposed an attosecond photoelectron interferometer based on strong-field photoelectron holography to resolve the tunneling ionization. Here, we show more details about how the complex ionization time of tunneling is retrieved with our scheme. We demonstrate that the Coulomb interaction, which is a tedious and complex problem in dealing with photoelectron interference in strong-field ionization, can be safely canceled in our scheme. This is further confirmed by performing our scheme for both the model atoms with short-range and Coulomb potentials. Additionally, the validity and accuracy of our scheme are confirmed by its application in different targets and different laser parameters. Our scheme provides a reliable and versatile method to resolve the time information of strong-field tunneling ionization.
Photoelectron holography in strong-field tunneling ionization is an efficient way to probe the structures and the ultrafast dynamics information of atoms and molecules. Manipulating the process of photoelectron holography is important for its application. Here, we study theoretically strong-field photoelectron holography in the spatially inhomogeneous field by solving the time-dependent Schr\"odinger equation. Our results show that the returning energy of the rescattering electron is greatly enhanced in the spatially inhomogeneous field, and the holographic interference pattern can be separated from other types of interference in the photoelectron momentum distribution. Moreover, our results show that the time window of tunneling ionization wherein the electron could be driven back to induce holography is broadened in the inhomogeneous field. These properties are beneficial for the application of photoelectron holography in probing the atomic and molecular structures and dynamics. The origin for these properties is analyzed with the classical trajectory model.
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.
Abstract Coherent superposition of several electronic states in molecules induces attosecond charge migration. We theoretically demonstrate a way to observe this attosecond charge migration in the asymmetric molecule HeH 2+ using strong-field photoelectron holography, complementary to our previous work (He M et al 2018 Phys. Rev. Lett. 120 , 133204) where the charge migration in the symmetric molecule was monitored. We disentangle the holographic interference from other types of interference in the photoelectron momentum distribution with the Fourier frequency filter method. By employing the holographic fringes originating from the ground state of HeH 2+ as a reference, we develop a feasible approach to visualize the charge migration in the asymmetric molecule with attosecond temporal resolution.
We study the dynamical photoelectron holography of an excited hydrogen atom with a strong midinfrared laser field using numerical solutions of the three-dimensional time-dependent Schr\"odinguer equation. A clear holographic interference pattern of first and high order (hologram) is recorded in the two-dimensional (2D) momentum distribution of the photoelectron. The patterns are well reproduced by additional quantitative calculations based on the Lippmann-Schwinger equation. Here, the high-order interference effect is linked to the multsicattering of low-momentum electrons driven by the midinfrared laser field prior to ejection. The phenomenon manifests by low-momentum structures in 2D momentum distributions and is found to be sensitive to the change of the optical carrier-envelope phase (CEP). By analyzing the temporal evolution of the buildup of the hologram, we show that this sensitivity results from the birth time of the continuum wave packet with an offset in time during the subcycle dynamics, thus encoding information about the ionization mechanism which is mapped into the CEP-resolved 2D momentum distributions and angle-resolved photoelectron spectra. It is indeed an indicator that the ejected electrons exhibit a memory of their birth-time. These findings suggest that the CEP-resolved photoelectron holography serves as a tool for a direct measurement of attosecond dynamics. Furthermore, the effects due to such multiple scattering electron paths can be used to design new atom interferometers to highlight mechanisms that require higher accuracy.