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Journal of Physics B Atomic Molecular and Optical Physics

Spectral manifestation of core coherence in photoionization

R. Grobe, Stanley L. Haan

Published Nov 28, 1994• 16 citations
Publisher

Abstract

Photoionization processes are considered for situations in which the laser frequency is close to a resonant frequency of the final positive ion core. It is predicted that resonant coupling within the ionic core can split photoelectron spectral peaks into doublets, with components separated by the effective Rabi frequency of the core. The possibility of superposing this final-state effect with previously studied effects involving laser-induced autoionizing states is considered. Specific predictions are made for the splitting of photoelectron peaks in photoionization of strontium.

DOI
10.1088/0953-4075/27/22/002

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Photoionization processes are considered for situations in which the laser frequency is close to a resonant frequency of the final positive ion core. It is predicted that resonant coupling within the ionic core can split photoelectron spectral peaks into doublets, with components separated by the effective Rabi frequency of the core. The possibility of superposing this final-state effect with previously studied effects involving laser-induced autoionizing states is considered. Specific predictions are made for the splitting of photoelectron peaks in photoionization of strontium.
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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.
The ionization of atoms with sequences of attosecond pulses gives rise to excited ionic states that are entangled with the emitted photoelectron. Still, the ionic ensemble preserves some coherence that can be controlled through the laser parameters. In helium, control of the 2s/2pHe+2s/2p\phantom{\rule{4pt}{0ex}}{\mathrm{He}}^{+}2s/2pHe+ coherence is mediated by the autoionizing states below the N=2N=2N=2 threshold [Phys. Rev. Res. 3, 023233 (2021)]. In the present work we study the role of the resonances both below and above the N=3N=3N=3 threshold on the coherence of the N=3He+N=3\phantom{\rule{4pt}{0ex}}{\mathrm{He}}^{+}N=3He+ ion, in the attosecond pump-probe ionization of the helium atom, which we simulate using the newstock ab initio code. Due to the fine-structure splitting of the N=3He+N=3{\mathrm{He}}^{+}N=3He+ level, the ionic dipole beats on a picosecond timescale. We show how, from the dipole beating, it is possible to reconstruct the polarization of the ion at its inception.
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.