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Journal of Physics B Atomic Molecular and Optical Physics

Imaging charge migration in the asymmetric molecule with the holographic interference in strong-field tunneling ionization

Mingrui He, Yueming Zhou, Jia Min Tan, Yang Li, Min Li, Peixiang Lu

Published Nov 12, 2018• 8 citations
Publisher

Abstract

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.

DOI
10.1088/1361-6455/aaf027

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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.
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 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.
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.
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.
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.
In a double-slit experiment with a bipartite system, the visibility of interference fringes depends on the availability of which-way information. Here, we report a Bell-like state of photoelectron and residual ion in the multiphoton dissociative ionization of the D2_22​ molecule. Evidence for entanglement is provided by the correlated emission directions of photoelectron and ion, which is observed using a COLTRIMS reaction microscope. In the presence of this correlation, the holographic interference fringes contained in the photoelectron momentum distributions are suppressed, indicating the existence of which-way information. The interference pattern persists when a single ionic state is populated and thus no which-way information is available. The experimental observations and conclusions are supported by the numerical solution of the electronic-nuclear time-dependent Schrödinger equation. Our work demonstrates that coincidence spectroscopy of ions and electrons is a powerful method for studying fundamental concepts of quantum information science within the context of ultrafast light-matter interactions.