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Physical Review A

Suppression of hole decoherence in ultrafast photoionization

Antonia Karamatskou, R. Esteban Goetz, Christiane P. Koch, Robin Santra

Published Apr 13, 2020• 4 citations
Publisher

Abstract

In simple one-photon ionization, decoherence occurs due to entanglement between ion and photoelectron. Therefore, the preparation of coherent superpositions of electronic eigenstates of the hole in the photoion is extremely difficult. We demonstrate for the xenon atom that the degree of electronic coherence of the photoion in attosecond photoionization can be enhanced if the influence of many-body interactions is properly controlled. A mechanism at low photon energies involving multiphoton ionization is found, suppressing the loss of coherence through ionization into the same photoelectron partial waves. The degree of coherence found between the $4{d}_{0}$ and $5s$ hole states is, on the one hand, limited by Auger decay of the $4{d}_{0}$ hole. On the other hand, increasing the population ratio such that a significant portion of the state is in a true superposition of both states renders the maximization of the degree of coherence difficult.

DOI
10.1103/physreva.101.043405

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Abstract Quantum coherence plays a fundamental role in the study and control of ultrafast dynamics in matter. In the case of photoionization, entanglement of the photoelectron with the ion is a well-known source of decoherence when only one of the particles is measured. Here, we investigate decoherence due to entanglement of the radial and angular degrees of freedom of the photoelectron. We study two-photon ionization via the 2s2p autoionizing state in He using high spectral resolution photoelectron interferometry. Combining experiment and theory, we show that the strong dipole coupling of the 2s2p and 2p 2^22 2 states results in the entanglement of the angular and radial degrees of freedom. This translates, in angle-integrated measurements, into a dynamic loss of coherence during autoionization. Graphic Abstract
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.
Coherent control provides a quantum interference based method for controlling atomic and molecular dynamics. We report two experimental observations of different ways to achieve such a control in atomic photoionization continuum. One is the photoionization of sodium atoms, initially prepared in the 3P1/2 excited state, by a non resonant three-photon interaction with 1064-nm laser light and by a one-photon interaction with the third-harmonic field, at 355 nm. Interference between the two transition paths allows the control of the total ionization rate by varying the relative phase of the laser fields. The second experiment is the observation of the modification of the ionization continua of xenon through laser induced continuum structure (LICS). The multiphoton radiative decay of the xenon ground state into the two electronic continua, that correspond to the two fine structure levels of the ground state of the xenon ion, is varied by electromagnetically embedding a bound state of the atom into the two continua. Both experiments are performed on an atomic beam apparatus which uses a time-of-flight spectrometer for energy analyzing the emitted photoelectrons.
Ultrafast multichannel single-photon ionization of Ar is investigated theoretically by a model calculation incorporating correlation between the photoelectron and photoion. It is shown that the coherent hole dynamics in Ar+ associated with a superposition of the spin–orbit states can be observed by using a Fourier-transform limited laser pulse for ionization, while the coherence is degraded or lost by chirped a laser pulse. We demonstrate that the coherent hole dynamics can be retrieved even in the case of ionization by a chirped laser pulse, by labeling the photoion dynamics with the counterpart photoelectron energy.
Ultrafast high harmonic beams provide new opportunities for coherently controlling excitation and ionization processes in atoms, molecules, and materials on attosecond time scales by employing multiphoton two-pathway electron-wave-packet quantum interferences. Here we use spectrally tailored and frequency tuned vacuum and extreme ultraviolet harmonic combs, together with two phase-locked infrared laser fields, to show how the total single and double photoionization yields of argon can be coherently modulated by controlling the relative phases of both optical and electronic-wave-packet quantum interferences. This Letter is the first to apply quantum control techniques to double photoionization, which is a fundamental process where a single, high-energy photon ionizes two electrons simultaneously from an atom.