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Journal of Physics B Atomic Molecular and Optical Physics

Photoelectron–photoion correlation in ultrafast multichannel photoionization of Ar

Ryuji Itakura, Mizuho Fushitani, Akiyoshi Hishikawa, Tokuei Sako

Published Sep 24, 2014• 3 citations
Publisher

Abstract

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.

DOI
10.1088/0953-4075/47/19/195602

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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.
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 4d04{d}_{0}4d0​ and 5s5s5s hole states is, on the one hand, limited by Auger decay of the 4d04{d}_{0}4d0​ 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.
The role of Rydberg autoionizing states in interfering one- and two-photon ionization paths is theoretically investigated in atomic Ar. The angularly resolved photoionization cross sections for each individual path is provided. By varying the relative optical phase between the two pulses the phase difference between the two interfering paths is extracted. The retrieved phase difference and the photoelectron angular distributions exhibit a strong dependence on the photon energy in the vicinity of the resonant states. In contrast to previous results obtained in atomic Ne, the phase difference features a smooth dependence with photoelectron emission angle.
To time-resolve attosecond electronic dynamics in general photoionization processes, the technique that retrieves the phase of emitted electronic wave packets without intercepting the interactions is essential. Here, we theoretically demonstrate a scheme that uses isolated attosecond pulses (IAPs) to achieve this goal. Our approach utilizes the coherent interference between the electronic wave packets of interest and the one produced by a subsequent IAP. It is shown that the photoelectron spectral phase that has eluded direct detection so far can be fully recovered from observable photoelectron spectra without perturbing the electron-release process under investigation. By further performing a time-frequency-like analysis on the photoelectron energy spectra with the spectral phase, we reveal the birth processes of photoelectrons in time and the association between electronic energy and birth time in strong-field ionization driven by circularly polarized laser pulses. The present work explores a promising application of IAPs for ultrafast measurement and opens a viable venue for investigating electronic dynamics with quantum phase information.
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.
Ultrafast atomic processes, such as excitation and ionization occurring on the femtosecond or shorter time scale, were explored by employing attosecond high-harmonic pulses. With the absorption of a suitable high-harmonic photon a He atom was ionized, or resonantly excited with further ionization by absorbing a number of infrared photons. The electron wave packets liberated by the two processes generated an interference containing the information on ultrafast atomic dynamics. The attosecond electron wave packet, including the phase, from the ground state was reconstructed first and, subsequently, that from the 1s3p state was retrieved by applying the holographic technique to the photoelectron spectra comprising the interference between the two ionization paths. The reconstructed electron wave packet revealed details of the ultrafast photoionization dynamics, such as the instantaneous two-photon ionization rate.