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The Journal of Physical Chemistry A

Control of Ion-Photoelectron Entanglement and Coherence Via Rabi Oscillations

Kenichi L. Ishikawa, Kevin Charles Prince, Kiyoshi Ueda

Published Dec 12, 2023• 15 citations
Publisher

Abstract

We report a theoretical investigation of photoionization by a pair of coherent, ultrashort, fundamental and second-harmonic extreme-ultraviolet pulses, where the photon energies are selected to yield the same photoelectron energy for ionization of two different subshells. This choice implies that the fundamental energy is equal to the difference in energy of the ionic states and that they are therefore coupled by the fundamental photon. By deriving analytical expressions using the essential-states approach, we show that this Rabi coupling creates coherence between the two photoelectron wave packets, which would otherwise be incoherent. We analyze how the coupling is affected by the parameters, such as relative phase, pulse width, delay between the two pulses, Rabi coupling strength, and photoelectron energy. Our discussion mostly considers Ne 2p and 2s photoionization, but it is generally valid for many other quantum systems where photoionization from two different shells is observed.

DOI
10.1021/acs.jpca.3c06781

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We report a theoretical investigation of photoionization by a pair of coherent, ultrashort, fundamental and second-harmonic extreme-ultraviolet pulses, where the photon energies are selected to yield the same photoelectron energy for ionization of two different subshells. This choice implies that the fundamental energy is equal to the difference in energy of the ionic states and that they are therefore coupled by the fundamental photon. By deriving analytical expressions using the essential-states approach, we show that this Rabi coupling creates coherence between the two photoelectron wave packets, which would otherwise be incoherent. We analyze how the coupling is affected by the parameters, such as relative phase, pulse width, delay between the two pulses, Rabi coupling strength, and photoelectron energy. Our discussion mostly considers Ne 2p and 2s photoionization, but it is generally valid for many other quantum systems where photoionization from two different shells is observed.
We present first-principles numerical simulations of photoionization in neon induced by bichromatic extreme ultraviolet pulses with frequencies ωωω and 2ω2ω2ω, specially chosen to make ωωω equal to the energy difference between the 2s2s2s and 2p2p2p subshells. This allows for the production of photoelectrons from the 2s2s2s shell by 2ω2ω2ω pulse and from the 2p2p2p shell by ωωω pulse with the same energy. Using the multi-configurational time-dependent Hartree-Fock method, we explore how Rabi coupling between subshells generates coherence between the corresponding photoelectron wave packets. Our \textit{ab initio} calculations confirm the analytical results derived from the essential-states approach in [K. L. Ishikawa, K. C. Prince, and K. Ueda, J. Phys. Chem. A 127, 10638 (2023)], validating the theoretical predictions. Although we focus on the Ne 2p2p2p and 2s2s2s subshells, our approach is applicable to a broad range of systems exhibiting photoionization from multiple subshells. The laser parameters employed in our simulations are available in modern Free Electron Lasers (FELs), and we anticipate that this work could stimulate experimental investigations using FELs to study ion-photoelectron coherence and entanglement.
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.
We make a theoretical investigation of photoionization of an H2{\mathrm{H}}_{2}H2​ molecule, induced by the irradiation of an ultrashort extreme ultraviolet (XUV) laser pulse. We consider a system composed of a photoelectron ejected from H2{\mathrm{H}}_{2}H2​ and the resultant H2+{{\mathrm{H}}_{2}}^{+}H2​+ as a bipartite system. In order to clarify how the interparticle correlations among two electrons and two protons in H2{\mathrm{H}}_{2}H2​ are reflected to the bipartite system, we examine the entanglement between the photoelectron and the vibrational states of H2+{{\mathrm{H}}_{2}}^{+}H2​+ as well as the coherence in the vibrational states of H2+{{\mathrm{H}}_{2}}^{+}H2​+ by simulating the photoionization process of one-dimensional H2{\mathrm{H}}_{2}H2​. In the simulation, we solve a time-dependent Schr\"odinger equation using a symmetry-adapted grid method. On the basis of the simulations with ten different sets of three parameters characterizing an ultrashort XUV laser pulse, i.e., the pulse duration, the wavelength, and the peak intensity, we show that the extent of the entanglement depends sensitively on the coherence in the vibrational states of H2+{{\mathrm{H}}_{2}}^{+}H2​+.
This thesis investigates quantum dynamics induced in atoms by ultrashort pulses of light. The work is motivated by recent developments in free-electron lasers, which generate ultrashort pulses of intense, coherent light and enable coherent control of quantum dynamics. We develop theoretical models to study the processes of absorption and emission in laser-atom interactions. Additionally, we study photoionisation, which creates an ion and an electron, and the entanglement that can be generated between these particles. Finally, we have investigated how the spontaneous decay of the ion induces entanglement transfer from the ion-electron pair to the electron-photon pair.This thesis compiles seven papers. Paper I investigates the absorption of light from an attosecond pulse by an atom in a prepared coherent superposition of states. We show how the evolution of the phase of the superposition wave packet influences the attosecond transient absorption spectra. Paper II predicts the existence of Mollow-like triplets in the absorption spectra of strongly coupled atoms. We establish the conditions for the pulse envelope under which this triplet pattern can be supported.Paper III studies two-photon Rabi oscillations, establishing which systems can sustain such dynamics. We find that a two-photon Rabi oscillating system can induce giant counter-rotating oscillations in the population dynamics, enabling investigations of physical effects beyond the rotating-wave approximation.Paper IV studies ionisation from an atom strongly coupled by a dichromatic field, where interference between the two frequency components shapes the temporal symmetry of the atomic dynamics, allowing for coherent control of the photoelectron distribution.Paper V considers an experiment performed at a Free-Electron Laser facility where a helium atom is ionised and the resulting ion is subsequently strongly coupled. The photoelectron spectra are theoretically reproduced and the entanglement between the ion and photoelectron is studied. Paper VI investigates how the entanglement in the ion--electron pair, generated via photoionisation followed by strong coupling, can be coherently controlled by harnessing the time symmetry of the pulse. We find that the observable manifestation of the entanglement can be altered in such a way that the electron energy becomes associated with the ionic state, allowing the entanglement to be detected via coincidence measurements. Paper VII investigates how quantum correlations between the ion and the electron can be coherently controlled by sequential strong coupling of the ion. We find that both the build-up of entanglement and its manifestation can be controlled, and we establish a quantitative measure of the amplitude entanglement that explains the dynamics in an intuitive way. Paper VIII studies the process of entanglement transfer induced by the spontaneous decay of the ion. We find that the ion--electron entanglement generated during the ultrashort interaction with the laser field is transferred to the electron--photon system over the much longer timescale of fluorescence.
We analyze theoretically the high intensity photoionization dynamics of a system with two atomic states resonantly coupled by coherent extreme ultraviolet laser radiation that also gives rise to the ionization. The ground state occupation of such a system is shown to exhibit damped Rabi oscillations. The corresponding ionization, which is responsible for the damping, scales almost linearly with the field intensity when the pulse length exceeds the Rabi period. For shorter pulses a quadratic scaling is found. The Rabi frequency is shifted compared to its value for an isolated two-level system. The shift increases with excitation intensity and can acquire a high percentage of the unrenormalized frequency at high intensities. Analytical results obtained within a simplified solvable model demonstrate that the damping and the shift both result from the coupling of the discrete states to the ionization continuum and are therefore closely related. Numerical simulations for a two-electron system reveal at high intensities the importance of off-resonant ionization channels.