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Journal of Physics B Atomic Molecular and Optical Physics

Three-dimensional photoelectron holography with trichromatic polarization-tailored laser pulses

D. Köhnke, Kevin Eickhoff, Tim Bayer, M. Wollenhaupt

Published Jul 26, 2022• 8 citations
Publisher

Abstract

Abstract We present a three-dimensional (3D) photoelectron wave packet holography scheme based on polarization-tailored trichromatic femtosecond laser pulses for the determination of quantum phases in atomic multiphoton ionization (MPI). Experimentally, we combine supercontinuum polarization pulse shaping with photoelectron tomography for the reconstruction of the 3D photoelectron momentum distribution (PMD). To demonstrate the 3D photoelectron holography scheme, we superimpose a sculptured wave packet encoding a relative continuum phase with a reference wave packet. In particular, we create a sculptured angular momentum superposition wave packet by (2 + 1) resonance-enhanced MPI of potassium atoms using a counter-rotating circularly polarized bichromatic pulse sequence. The sculptured wave packet, consisting of states with different orbital angular momentum quantum numbers, interferes with the reference wave packet generated by direct three-photon ionization with a circularly polarized pulse of the third color. Depending on the circularity of the reference pulse, interference of both wave packets gives rise to 3D photoelectron holograms with c 2 or c 4 rotational symmetry in the laser polarization plane, i.e., in the azimuthal direction. In the polar direction, the azimuthal interference pattern undergoes a phase-shift revealing the relative quantum phase between the p- and f-type continuum partial waves in the sculptured wave packet. We determine the relative continuum phase by fitting the parameters of an analytical model of the hologram to the measured 3D PMD and confirm the result by direct extraction of the continuum phase difference from the polar-angle-dependent azimuthal phase-shift of the photoelectron angular distribution.

DOI
10.1088/1361-6455/ac845f

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Abstract We present a three-dimensional (3D) photoelectron wave packet holography scheme based on polarization-tailored trichromatic femtosecond laser pulses for the determination of quantum phases in atomic multiphoton ionization (MPI). Experimentally, we combine supercontinuum polarization pulse shaping with photoelectron tomography for the reconstruction of the 3D photoelectron momentum distribution (PMD). To demonstrate the 3D photoelectron holography scheme, we superimpose a sculptured wave packet encoding a relative continuum phase with a reference wave packet. In particular, we create a sculptured angular momentum superposition wave packet by (2 + 1) resonance-enhanced MPI of potassium atoms using a counter-rotating circularly polarized bichromatic pulse sequence. The sculptured wave packet, consisting of states with different orbital angular momentum quantum numbers, interferes with the reference wave packet generated by direct three-photon ionization with a circularly polarized pulse of the third color. Depending on the circularity of the reference pulse, interference of both wave packets gives rise to 3D photoelectron holograms with c 2 or c 4 rotational symmetry in the laser polarization plane, i.e., in the azimuthal direction. In the polar direction, the azimuthal interference pattern undergoes a phase-shift revealing the relative quantum phase between the p- and f-type continuum partial waves in the sculptured wave packet. We determine the relative continuum phase by fitting the parameters of an analytical model of the hologram to the measured 3D PMD and confirm the result by direct extraction of the continuum phase difference from the polar-angle-dependent azimuthal phase-shift of the photoelectron angular distribution.
We present the unambiguous determination of quantum phases in the multiphoton ionization (MPI) of potassium atoms by using a multichannel photoelectron interferometry scheme based on trichromatic pulse shaping. The colors of the laser field are chosen to produce three energetically separated photoelectron interferograms in the continuum. While the red pulse is two-photon resonant with the 3d3d3d state resulting in a (2+1)(2+1)(2+1) resonance-enhanced MPI (REMPI), a (1+2)(1+2)(1+2) REMPI occurs via the nonresonant intermediate 4p4p4p state with an initial green or blue pulse. We show that ionization via a nonresonant intermediate state lifts the degeneracy of photoelectron interferograms from pathways consisting of permutations of the colors. The analysis of the interferograms reveals a phase shift of $\ifmmode\pm\else\textpm\fi{}\ensuremath{\pi}/2$ depending on the sign of the detunings in the (1+2)(1+2)(1+2) REMPI pathways. In addition, we demonstrate that the photoionization time delay in the resonant (2+1)(2+1)(2+1) REMPI pathway gives rise to a linear spectral phase in the photoelectron spectra. Insights into the underlying MPI processes are gained through an analytic perturbative description and numerical simulations of a trichromatic driven three-level system coupled to the continuum.
Polarization-tailored bichromatic femtosecond laser fields with cycloidal polarization profiles have emerged as a powerful tool for coherent control of quantum processes. We present an optical scheme to create and manipulate three-dimensional free electron wave packets with arbitrary rotational symmetry by combining advanced supercontinuum pulse shaping with high resolution photoelectron tomography. Here we use carrier-envelope phase-stable polarization-tailored bichromatic (3ω:4ω) counter- and corotating femtosecond laser pulses to generate 7-fold rotational symmetric and asymmetric photoelectron momentum distributions by multiphoton ionization of sodium atoms. To elucidate the physical mechanisms, we investigate the interplay between the symmetry properties of the driving field and the resulting electron wave packets by varying the optical field parameters. Our results show that the symmetry properties of electron wave packets are not fully determined by the field symmetry, but completely described by multipath quantum interference of states with different angular momenta.
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We combine bichromatic polarization pulse shaping with photoelectron imaging tomography for time-resolved spatial imaging of ultrafast spin–orbit wave packet (SOWP) dynamics in atoms. Polarization-shaped two-color pump-probe sequences are generated by spectral amplitude and phase modulation of a femtosecond input pulse and used to excite SOWPs in the potassium fine-structure doublet. By selecting different spectral bands for pump and probe pulse, we achieve interference-free detection of the spatiotemporal SOWP dynamics. Using tomographic techniques, we reconstruct the three-dimensional photoelectron momentum distribution (3D-ED) created by the probe pulse. Time-resolved measurement of the 3D-ED reveals the orbital realignment dynamics induced by spin–orbit interaction in the neutral atom.
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.