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Physical Review A

Reconstruction of attosecond beating by interference of two-photon transitions on the lithium atom with Rabi oscillations

Yijie Liao, Yueming Zhou, Liang-Wen Pi, Jintai Liang, Qinghua Ke, Yong Zhao, Min Li, Peixiang Lu

Published Jun 24, 2022• 12 citations
Publisher

Abstract

We present numerical simulations of the reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) on lithium by solving the three-dimensional time-dependent Schr\"odinger equation. In our scheme, the infrared (IR) field couples the $2s$ and $2p$ states of lithium and leads to the Rabi oscillations of populations between these two states. We analyzed the RABBITT phases of the two peaks in the Rabi-oscillation-induced Autler-Townes splittings. Our results show that the relative phase between these two peaks changes with the photoelectron energy and depends on the intensity of the IR field. Moreover, in the angle-resolved RABBITT measurement, the phases of the two peaks depend differently on the emission angle of photoelectrons. These behaviors are traced back to the different initial phases of the electron wave packets emitted from the dressed $2p$ states and the competition among different ionization channels.

DOI
10.1103/physreva.105.063110

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We present numerical simulations of the reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) on lithium by solving the three-dimensional time-dependent Schr"odinger equation. In our scheme, the infrared (IR) field couples the 2s2s2s and 2p2p2p states of lithium and leads to the Rabi oscillations of populations between these two states. We analyzed the RABBITT phases of the two peaks in the Rabi-oscillation-induced Autler-Townes splittings. Our results show that the relative phase between these two peaks changes with the photoelectron energy and depends on the intensity of the IR field. Moreover, in the angle-resolved RABBITT measurement, the phases of the two peaks depend differently on the emission angle of photoelectrons. These behaviors are traced back to the different initial phases of the electron wave packets emitted from the dressed 2p2p2p states and the competition among different ionization channels.
We utilize the reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) technique to study the phase of a Rabi-cycling atom using circularly polarized extreme ultraviolet and infrared fields, where the infrared field induces Rabi oscillations between the 2s2s2s and 2p2p2p states of lithium. Autler-Townes splittings are observed in sidebands of the photoelectron spectra and the relative phases of outgoing electron wave packets are retrieved from the azimuthal angle. In this RABBITT scheme, more ionization pathways beyond the usual two-photon pathways are required. Our results show that the polar-angle-integrated and polar-angle-resolved RABBITT phases have different behaviors when the extreme ultraviolet and infrared fields have co- and counter-rotating circular polarizations, which are traced back to the different ionization channels according to the selection rules in these two cases and their competition relying on the propensity rule in laser-assisted photoionization.
We utilize the reconstruction of attosecond beating by interference of two-photon transitions (RABBIT) technique to study the phase of a Rabi-cycling atom using circularly polarized extreme ultraviolet and infrared (IR) fields, where the IR field induces Rabi oscillations between the 2s and 2p states of lithium. Autler-Townes splittings are observed in sidebands of the photoelectron spectra and the relative phases of outgoing electron wave packets are retrieved from the azimuthal angle. In this RABBIT scheme, more ionization pathways beyond the usual two-photon pathways are required. Our results show that the polar-angle-integrated and polar-angle-resolved RABBIT phases have different behaviors when the XUV and IR fields have co- and counter-rotating circular polarizations, which are traced back to the different ionization channels according to the selection rules in these two cases and their competition relying on the propensity rule in laser-assisted photoionization.
Reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) is a technique that can be used to determine the phases of atomic transition elements in photoionization processes. In the traditional RABBITT scheme, the so-called asymptotic approximation considers the measured phase as a sum of the Wigner phase linked to a single-photon ionization process and the continuum-continuum phase associated with further single-photon transitions in the continuum. In this paper, we extend the asymptotic approximation to multi-sideband RABBITT schemes. The predictions from this approximation are then compared with results obtained by an ab initio calculation based on solving the time-dependent Schr\"odinger equation for atomic hydrogen.
The reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) method is a leading technique for time-resolved investigation of photoionization processes. Interpretation of RABBITT spectra is limited to a lowest-order description, while new variants of the technique necessitate higher intensity infrared fields where this description breaks down. Here, we present an extension of RABBITT theory which can account for higher-order processes (RABBITT-HOP), and demonstrate RABBITT-HOP's ability to predict and describe higher-order processes through simulation of a RABBITT experiment targeting the high-lying 1 s n p Rydberg series of helium. We demonstrate that the signature line shape imparted by the resonances in the 2 ω phase of the lowest sideband can also be observed in the 2 ω phase of the next mainband, as well as in the 4 ω phases of the next sideband and mainband—each with additional phase shifts predicted under RABBITT-HOP. Repeating this analysis for a range of infrared intensities, we determine the lower limits of intensities required for these higher-order processes to become observable and upper limits beyond which nonperturbative effects begin to dominate. This new theoretical framework forms a much-needed basis for accurate interpretation of RABBITT spectra in experiments involving more intense fields, and paves the way for the development of new RABBITT-like techniques which take advantage of this new understanding of how atomic resonance effects may be propagated beyond their nearest sideband.
Abstract We study the three-photon ionization of atomic lithium by intense, short light pulses, via numerically solving the time-dependent Schrödinger equation. Two-photon Rabi oscillations are induced between the 2s and 4s states, which are damped due to single-photon ionization to the p continuum. Developing a minimal three-level model, we analyze the spectral features of the Autler–Townes (AT) doublet that is formed upon the resonant coupling with the laser pulse. Furthermore, we show that this 2 s →→ 4 s → p c o n t i n u u m pathway is the dominant process, if the duration of the laser pulse exceeds a certain value. For shorter pulses, ionization through the 2p state ( 2 s → 2 p → 4 d → f c o n t i n u u m ) gradually becomes the dominant process, provided that the pulse is strong enough to induce several Rabi floppings. Here, we trace the competition of these ionization pathways by observing the structural changes in the shape of the AT doublet.
The reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) setup is theoretically studied for various combinations of extreme ultraviolet and infrared (IR) field components polarization: ``linear+linear\mathrm{linear}+\mathrm{linear}linear+linear,'' ``linear+circular\mathrm{linear}+\mathrm{circular}linear+circular'' with crossed propagation directions, and ``circular+circular\mathrm{circular}+\mathrm{circular}circular+circular'' with parallel propagation directions. We examine the general properties of photoelectron angular distributions and their response to the variation of the IR pulse delay. Numerical simulations are performed for the neon valence shell ionization into the structureless continuum using two approaches: time-dependent perturbation theory and the solution of amplitude rate equations. To distinguish between ``geometrical'' governed by fields polarization and spectroscopic features, we provide an additional analysis for the case of sss-shell ionization.