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Журнал Экспериментальной и Теоретической Физики

Attosecond Interferometry Involving Discrete States

Maria M. Popova, S. N. Yudin, Грызлова Елена Владимировна, Maksim D. Kiselev, A. N Grum-Grzhimaylo

Published Mar 15, 2023• 2 citations
Publisher

Abstract

In the paper we theoretically investigate the features of RABBITT (Reconstruction of Attosecond Beating By Interference of Two-photon Transitions) spectroscopy under conditions when transitions through discrete spectrum states play a significant role. Two approaches are applied in the article: the numerical solution of rate equations with continuum discretization and the perturbation theory up to the third order in amplitude. Both approaches use transition matrix elements and photoionization amplitudes obtained by the high-precision R-matrix method. Within the framework of these approaches, photoelectron spectra, the amplitude and phase of RABBITT oscillations were obtained, and the effect of the seed optical field intensity and detuning from a resonance upon excitation of discrete states was studied.

DOI
10.31857/s004445102303001x

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In the paper we theoretically investigate the features of RABBITT (Reconstruction of Attosecond Beating By Interference of Two-photon Transitions) spectroscopy under conditions when transitions through discrete spectrum states play a significant role. Two approaches are applied in the article: the numerical solution of rate equations with continuum discretization and the perturbation theory up to the third order in amplitude. Both approaches use transition matrix elements and photoionization amplitudes obtained by the high-precision R-matrix method. Within the framework of these approaches, photoelectron spectra, the amplitude and phase of RABBITT oscillations were obtained, and the effect of the seed optical field intensity and detuning from a resonance upon excitation of discrete states was studied.
In the paper we theoretically investigate the features of RABBITT (Reconstruction of Attosecond Beating By Interference of Two-photon Transitions) spectroscopy under conditions when transitions through discrete spectrum states play a significant role. Two approaches are applied in the article: the numerical solution of rate equations with continuum discretization and the perturbation theory up to the third order in amplitude. Both approaches use transition matrix elements and photoionization amplitudes obtained by the high-precision R-matrix method. Within the framework of these approaches, photoelectron spectra, the amplitude and phase of RABBITT oscillations were obtained, and the effect of the seed optical field intensity and detuning from a resonance upon excitation of discrete states was studied.
Abstract In the paper we present the angular distributions of photoelectrons in ionization of neon atom by a field of several multiple frequencies. The considered setup is referred to the RABBITT (reconstruction of attosecond beating by interference of two-photon transitions) spectroscopy under condition that the field frequencies are selected in such a way that resonant transitions through discrete states play an important role. The role of the phase of the seeding infrared field on the angular distributions of photoemission is analyzed. A significant difference in the anisotropy parameters at the near-threshold sideband caused by transitions through discrete states is shown. Two methods are compared: numerical solution of the rate equations with continuum discretization and third-order perturbation theory.
In the paper we present the angular distributions of photoelectrons in ionization of neon atom by a field of several multiple frequencies. The considered setup is refered to the RABBITT (Reconstruction of Attosecond Beating By Interference of Two-photon Transitions) spectroscopy under condition that the field frequencies are selected in such a way that resonant transitions through discrete states play an important role. The role of the phase of the seed infrared field on the angular distributions of photoemission is analyzed. A significant difference in the anisotropy parameters at the near-threshold sideband caused by transitions through discrete states is shown. Two methods are compared: numerical solution of rate equations with continuum discretization and third-order perturbation theory.
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.
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.
Following up on a previous paper on two-color photoionization of Ar(3p) [D. Bharti , ], we present measurements and calculations for a modified three-sideband (3-SB) version of the reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) configuration applied to He(1s) . The 3-SB RABBITT approach allows us to explore interference effects between pathways involving different orders of transitions within the continuum. The relative differences in the retrieved oscillation phases of the three sidebands provide insights into the continuum-continuum transitions. The ground state of helium has zero orbital angular momentum, which simplifies the analysis of oscillation phases and their angle dependence within the three sidebands. We find qualitative agreement between our experimental results and the theoretical predictions for many cases but also observe some significant quantitative discrepancies. Published by the American Physical Society 2024