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arXiv:1505.00035 · Journal of Physics B Atomic Molecular and Optical Physics

Coherent control of photoelectron wavepacket angular interferograms

Paul Hockett, M. Wollenhaupt, Thomas Baumert

Published Sep 23, 2015• 10 citations
arXivHTMLPDF

Abstract

Coherent control over photoelectron wavepackets, via the use of polarization-shaped laser pulses, can be understood as a time and polarization-multiplexed process, where the final (time-integrated) observable coherently samples all instantaneous states of the light–matter interaction. In this work, we investigate this multiplexing via computation of the observable photoelectron angular interferograms resulting from multi-photon atomic ionization with polarization-shaped laser pulses. We consider the polarization sensitivity of both the instantaneous and cumulative continuum wavefunction; the nature of the coherent control over the resultant photoelectron interferogram is thus explored in detail. Based on this understanding, the use of coherent control with polarization-shaped pulses as a methodology for a highly multiplexed coherent quantum metrology is also investigated, and defined in terms of the information content of the observable.

DOI
10.1088/0953-4075/48/21/214004

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•Jan 1, 1995•0 citations
Coherent control over photoelectron wavepackets, via the use of polarization-shaped laser pulses, can be understood as a time and polarization-multiplexed process, where the final (time-integrated) observable coherently samples all instantaneous states of the light–matter interaction. In this work, we investigate this multiplexing via computation of the observable photoelectron angular interferograms resulting from multi-photon atomic ionization with polarization-shaped laser pulses. We consider the polarization sensitivity of both the instantaneous and cumulative continuum wavefunction; the nature of the coherent control over the resultant photoelectron interferogram is thus explored in detail. Based on this understanding, the use of coherent control with polarization-shaped pulses as a methodology for a highly multiplexed coherent quantum metrology is also investigated, and defined in terms of the information content of the observable.
The feasibility of complete photoionization experiments, in which the full set of photoionization matrix elements is determined, using multiphoton ionization schemes with polarization-shaped pulses has recently been demonstrated [P. Hockett et al., Phys. Rev. Lett. 112, 223001 (2014)]. Here we extend our previous work to discuss further details of the numerics and analysis methodology utilized and compare the results directly to new tomographic photoelectron measurements, which provide a more sensitive test of the validity of the results. In so doing we discuss in detail the physics of the photoionization process and suggest various avenues and prospects for this coherent multiplexing methodology.
Photoelectron interferograms, manifested in photoelectron angular distributions (PADs), are high-information, coherent observables. In order to obtain the maximum information from angle-resolved photoionization experiments it is desirable to record the full, three-dimensional (3D), photoelectron momentum distribution. Here we apply tomographic reconstruction techniques to obtain such 3D distributions from multiphoton ionization of potassium atoms, and fully analyze the energy and angular content of the 3D data. The PADs obtained as a function of energy indicate good agreement with previous 2D data and detailed analysis [Hockett et al., Phys. Rev. Lett. 112, 223001 (2014)] concerning the main spectral features, but also indicate unexpected symmetry breaking in certain regions of momentum space, thus revealing additional continuum interferences which cannot otherwise be observed. These observations reflect the presence of additional ionization pathways and, most generally, illustrate the power of maximum-information measurements of coherent observables for quantum metrology of complex systems.
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.
Quantitative control and measurement of quantum entanglement are essential for advancing quantum technologies. Photoionization induced by ultrashort laser pulses provides a unique platform for studying entanglement between photoelectrons and residual ions, representing one of the most intriguing quantum phenomena in attosecond physics. Although extensive studies have focused on the coherence properties within either the emitted electrons or the ions individually, the electron-ion entanglement has remained largely unexplored. In this work, we bridge this gap by investigating the resonance-enhanced multiphoton ionization of argon atoms driven by two time-delayed ultrashort ultraviolet pulses. Employing state-of-the-art first-principles multi-electron simulations, we demonstrate the ability to reconstruct and precisely manipulate the purity of electron quantum states through detailed analysis of the photoelectron angular distributions. Our results reveal distinct scattering-phase differences among various electron configurations within the same partial wave channel, providing unequivocal evidence of electron-ion correlation and entanglement. With the fast development of free-electron lasers, this study establishes an experimentally feasible framework for directly controlling quantum entanglement in ultrafast ionization processes, offering new insights and powerful methodologies for exploring complex electron dynamics in many-electron systems.
The influence of laser-induced continuum structure on the angular distribution of photoelectrons is studied in the femtosecond time domain by direct numerical solution of the time-dependent Schrodinger equation. Control of the photoelectron angular distribution is demonstrated for the hydrogen atom by coherent population transfer from the initial S-state to an excited D-state via the p-continuum and further ionization into the f-continuum states. A direct optimization procedure is used to find a domain of laser parameters, for which the efficiency of the control with respect to the time delay and energy detuning between the laser pulses is maximized.
This work presents the results of an effort to use unique forms of optical radiation to better probe and control matter. Results are presented of a study of intense field photo-ionization of krypton and xenon in a two-color field. The use of a two-color field provides a valuable probe, the relative optical phase, into the dynamics of the ionization process. It is found that phase dependent tunneling character is preserved even though the photoelectron spectra indicate that the experiments performed were well into the multi-photon regime of ionization. Evidence for core scattering of the departing electrons is seen in the changes to the phase dependent spectra as the polarization of the exciting light is varied from linear to slightly elliptical. To further control the optical field, a pulse shaper was constructed using liquid crystal modulators that allowed either spectral phase or spectral amplitude shaping of a short pulse. The results were characterized using cross-correlations. The shaped light was then subsequently amplified in a chirped pulse amplifier. This light was characterized using Frequency Resolved Optical Gating, a newly developed technique for the complete determination of the optical field in a short pulse. The shaped pulses were then used to tailor atomic radial wavepackets in cesium. The evolution of the wavepackets was monitored by measuring atomic auto-interferograms for the case of amplitude shaping, which was used to control the atomic states excited. Cross-interferograms were used for phase shaping, which was used to select the initial phase of the atomic states. The cross-interferograms required the simultaneous amplification of a shaped and an unshaped pulse in our amplifier.