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Physical Review A

Entanglement and coherence in photoionization of H2 by an ultrashort XUV laser pulse

Takanori Nishi, Erik Lötstedt, Kaoru Yamanouchi

Published Jul 30, 2019• 29 citations
Publisher

Abstract

We make a theoretical investigation of photoionization of an ${\mathrm{H}}_{2}$ molecule, induced by the irradiation of an ultrashort extreme ultraviolet (XUV) laser pulse. We consider a system composed of a photoelectron ejected from ${\mathrm{H}}_{2}$ and the resultant ${{\mathrm{H}}_{2}}^{+}$ as a bipartite system. In order to clarify how the interparticle correlations among two electrons and two protons in ${\mathrm{H}}_{2}$ are reflected to the bipartite system, we examine the entanglement between the photoelectron and the vibrational states of ${{\mathrm{H}}_{2}}^{+}$ as well as the coherence in the vibrational states of ${{\mathrm{H}}_{2}}^{+}$ by simulating the photoionization process of one-dimensional ${\mathrm{H}}_{2}$. 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 ${{\mathrm{H}}_{2}}^{+}$.

DOI
10.1103/physreva.100.013421

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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​+.
We present a theoretical study on the response of a hydrogen atom to the simultaneous irradiation of ultrashort extreme ultraviolet (xuv) and laser pulses. The calculation is based on the time-dependent Schr\"odinger equation. The xuv photon energy is chosen to induce the $1s\ensuremath{-}2p$ transition. Our results indicate that we can transiently reduce the xuv absorption and change the atomic state within a few femtoseconds by injecting a femtosecond laser pulse. The laser-induced photoemission is affected by the addition of an xuv pulse and its yield depends much on the temporal overlap of the two pulses.
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 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.
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.
Quantum mechanics forbids us to describe a particle, once it correlates with another, as an individual physical object whose complete set of properties can be solely determined.Such correlations play one of the most important roles in understanding quantum phenomena such as non-adiabatic transitions in molecular dissociation, quantum teleportation, and Bose-Einstein condensate.This dissertation theoretically explores several phenomena to reveal the role of quantum correlations in molecular systems.Specifically, it studies the photoionization of H 2 and unambiguously evaluates the correlation between the photoelectron and H + 2 in terms of entanglement between the two particles.The correlation among the vibrational states of H + 2 is evaluated in terms of coherence and the relation with entanglement is studied.The ultrafast vibrational motion of H + 2 and its dependence on the photoelectron is analysed and the origin of this correlation is ascribed to the non-locality of the wave function.Moreover, the experimental scheme to extract the correlation effect from the vibrational motion of H + 2 using the sequence of ultrashort laser pulses is proposed.The correlation between a molecule and photons in a plasmonic nanocavity is also studied.This system has been attracting attention due to its potential use in quantum information and in the control of chemical reactions, and the analytical and numerical methods for describing the molecular dynamics in such a system are formulated.
Controlling coherence and interference of quantum states is one of the central goals in quantum science. Different from energetically discrete quantum states, however, it remains a demanding task to visualize coherent properties of degenerate states (e.g., magnetic sublevels). It becomes further inaccessible in the absence of an external perturbation (e.g., Zeeman effect). Here, we present a theoretical analysis of all-optical control of degenerate magnetic states in the molecular hydrogen ion, $ {\rm H}_2^ + $H2+, by using two time-delayed co- and counterrotating circularly polarized attosecond extreme-ultraviolet (XUV) pulses. We perform accurate simulations to examine this model by solving the three-dimensional time-dependent Schrödinger equation. A counterintuitive phenomenon of quantum interference between degenerate magnetic sublevels appears in the time-dependent electronic probability density, which is observable by using x-ray-induced transient angular and energy-resolved photoelectron spectra. This work provides an insight into quantum interference of electron dynamics inside molecules at the quantum degeneracy level.