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Physical Review A

Timing angular momentum transfer for parity-unfavored transitions in multiphoton ionization

Meng Han, Hao Liang, Peipei Ge, Yiqi Fang, Zhenning Guo, Xiaoyang Yu, Yongkai Deng, Liang-You Peng, Qihuang Gong, Yunquan Liu

Published Dec 3, 2020• 5 citations
Publisher

Abstract

When a bound electron is photoionized from an atom or molecule, the remaining multielectron ion with excess internal energy will relax towards lower-energy states. The subsequent transverse angular momentum transfer between the parent ion and the ejected electron can lead to an electron parity-unfavored transition. Here we perform a self-calibrated timing experiment to measure the time delay of the angular momentum transfer of parity-unfavored transitions during the multiphoton ionization. We use a strong linearly polarized 400-nm light field to trigger a parity-unfavored transition in the channel of the spin-orbit excited ionic state of krypton atoms and then selectively probe the phases of the electron wave functions with different magnetic quantum numbers with a weak parallelly (orthogonally) polarized 800-nm light field. The parallel and orthogonal probes serve as the start and the stop of a stopwatch, respectively. Hence, this allows us to access the characteristic time of such an ultrafast intra-atom multielectron process.

DOI
10.1103/physreva.102.061101

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When a bound electron is photoionized from an atom or molecule, the remaining multielectron ion with excess internal energy will relax towards lower-energy states. The subsequent transverse angular momentum transfer between the parent ion and the ejected electron can lead to an electron parity-unfavored transition. Here we perform a self-calibrated timing experiment to measure the time delay of the angular momentum transfer of parity-unfavored transitions during the multiphoton ionization. We use a strong linearly polarized 400-nm light field to trigger a parity-unfavored transition in the channel of the spin-orbit excited ionic state of krypton atoms and then selectively probe the phases of the electron wave functions with different magnetic quantum numbers with a weak parallelly (orthogonally) polarized 800-nm light field. The parallel and orthogonal probes serve as the start and the stop of a stopwatch, respectively. Hence, this allows us to access the characteristic time of such an ultrafast intra-atom multielectron process.
We observe the parity-unfavored photoelectron emission in multiphoton single ionization of krypton atoms in an intense ultraviolet laser field. With systematic experiments of successively varying the light ellipticity and intensity, we identify that this parity-unfavored emission is associated with the first excited ionic state via a resonant pathway. We reveal an abnormal Coulomb asymmetry of the parity-unfavored photoelectron emission in elliptically polarized fields when the ellipticity is less than 0.3. The simulation using the time-dependent Schr\"odinger equation based on single-active-electron approximation fails to reproduce the experiment. We attribute the experimental observations to the angular momentum correlation between the resonantly excited electron and the spin-orbit excited ion. Our results demonstrate that the well-known picture of the angular momentum transfer in multiphoton ionization is broken and instead that the electron shares the spin angular momenta of photons with the ion as an effect of electron correlations.
Single-photon ionization of an atom or molecule can be subdivided into parity-favored and -unfavored transitions, the latter characterized by electron emission, preferentially perpendicular to the electric vector. The nonresonant existence of these transitions is shown experimentally and studied over an extended energy range for a variety of satellite transitions in atomic argon. The spectra exhibit several clearly resolved satellite lines with strongly negative \ensuremath{\beta} values close to -1, independent of the photon energy. The results confirm the corresponding predictions of angular-momentum transfer theory.
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.
The precession of orbital and spin angular momentum vectors has been observed in a pump-probe study of the 4P fine-structure states of atomic potassium. A femtosecond pump pulse prepared a coherent superposition of the two fine-structure components. A time-delayed probe pulse then ionized the system after it had been allowed to evolve freely. Oscillations recorded in the ion signal reflect the evolution of the orientation of the orbital and spin angular momentum due to spin-orbit coupling. This interpretation gives physical insight into the cause of the half-period phase shift observed when the relative polarizations of the laser pulses were changed from parallel to perpendicular. Finally, it is shown that these changes in the orientation of the spin momentum vector of the system can be utilized to produce highly spin-polarized free electrons on the femtosecond scale
Ultrafast spectroscopy with attosecond resolution has enabled the real time observation of ultrafast electron dynamics in atoms, molecules and solids. These experiments employ attosecond pulses or pulse trains and explore dynamical processes in a pump-probe scheme that is selectively sensitive to electronic state of matter via photoelectron or XUV absorption spectroscopy or that includes changes of the ionic state detected via photo-ion mass spectrometry. Here, we demonstrate how the implementation of combined photo-ion and absorption spectroscopy with attosecond resolution enables tracking the complex multidimensional excitation and decay cascade of an Auger auto-ionization process of a few femtoseconds in highly excited krypton. In tandem with theory, our study reveals the role of intermediate electronic states in the formation of multiply charged ions. Amplitude tuning of a dressing laser field addresses different groups of decay channels and allows exerting temporal and quantitative control over the ionization dynamics in rare gas atoms.
Strong field ionization injects a transient vacancy in the atom which is entangled to the outgoing photoelectron. When the electron is finally detached, the ion is populated at different excited states with part of coherence information lost. The preserved coherence of matter after interacting with intense short pulses has important consequences on the subsequent nonequilibrium evolution and energy relaxation. Here we employ attosecond transient absorption spectroscopy to measure the time-delay of resonant transitions of krypton vacancy during their creation. We have observed that the absorptions by the two spin-orbit split states are modulated at different paces when varying the time-delay between the near-infrared pumping pulse and the attosecond probing pulse. It is shown that the coupling of the ions with the remaining field leads to a suppression of ionic coherence. Comparison between theory and experiments uncovers that coherent Raman coupling induces time-delay between the resonant absorptions, which provides insight into laser-ion interactions enriching attosecond chronoscopy.