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Two-photon ionization of many-electron atoms

J. Hofbrucker

Published Jan 1, 2020• 0 citations
Publisher

Abstract

Until recently, the nonlinear interaction between light and matter has been restricted to only low photon energies produced by optical lasers. However, about a decade ago, the rise of free-electron laser facilities revolutionized the field of nonlinear light-matter interaction by delivering intense high-energy light pulses. Today, such lasers are used for research in materials science, chemical technology, biophysical science, solid state physics as well as fundamental research. It is the new experimental possibilities provided by free-electron lasers that motivated the work presented in this thesis. Two-photon ionization process is one of the simplest nonlinear interactions in which absorption of two photons by an atom (or a molecule) leads to promoting one of its bound electrons to continuum. This work presents studies of two-photon ionization of neutral atoms. After a brief historical introduction to the topic of nonlinear light-matter interaction, the density matrix describing the state of an atom and a photoelectron following two-photon ionization is derived. In each successive chapter, part of this density matrix is used to obtain characteristic quantities such as total two-photon ionization cross section, photoelectron angular distributions, ion polarization or degree of polarization of fluorescence photon produced by subsequent decay of the photoion. Physical properties of these quantities are studied and intriguing phenomena, such as elliptical dichroism, polarization transfer as well as relativistic and screening effects are investigated.

DOI
10.22032/dbt.44410

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Elliptical dichroism is known in atomic photoionization as the difference in the photoelectron angular distributions produced in nonlinear ionization of atoms by left- and right-handed elliptically polarized light. We theoretically demonstrate that the maximum dichroism |Δ_{ED}|=1 always appears in two-photon ionization of any atom if the photon energy is tuned in so that the electron emission is dominantly determined by two intermediate resonances. We propose the two-photon ionization of atomic helium in order to demonstrate this remarkable phenomenon. The maximum elliptical dichroism could be used as a sensitive tool for analyzing the polarization state of photon beams produced by free-electron lasers.
Merging two subfields, collisions and spectroscopy, this book presents the latest research proposals, innovative experiments and fresh ideas. Topics considered include radiative collision induced electron continuum-continuum scattering; models of laser-induced chemical reactions; experimental studies of laser-induced ionizing collisions; laser photodissociation of Na/sub 2/ + ions produced by laser resonant ionization of Na vapor; steady-state electron-atom collision in a laser field; conditions for the observation of the predicted splitting of the laser assisted electron impact of the differential cross section of atoms; transitions between resonances; some proposals for experiments; above-threshold multiphoton ionization; observability of optical collisions in the frequency and the time domain; laser switched collisions - a diagrammatical approach; polarization of atomic fluorescence excited by molecular photodissociation; multiphoton selective excitation; on the role of chaotic dynamics with many basins of attraction; predissociation in a strong electromagnetic field; theory of double resonance; and coherent excitation of polyatomic molecules up to highly excited vibrational states by laser light.
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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.