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arXiv:2011.02989 · Physical Review A

Decomposition of the transition phase in multi-sideband schemes for reconstruction of attosecond beating by interference of two-photon transitions

Divya Bharti, David Atri-Schuller, Gavin Menning, Kathryn R. Hamilton, R. Moshammer, Thomas Pfeifer, Nicolas Douguet, Klaus Bartschat, Anne Harth

Published Feb 26, 2021• 39 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physreva.103.022834

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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.
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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.
In measurements of relative phases in photoionization processes, the contribution of continuum-continuum (CC) couplings to the atomic (Wigner) phases, corresponding to attosecond time delays, is currently accounted for only by theoretical models. Here, we introduce a measurement scheme that is sensitive to phase differences of CC transitions after photoionization in the presence of an optical field. The method allows us to separate CC transitions from the ionization process and can help in testing existing theoretical models. It is based on a multicolor interferometer, similar to the RABBITT (reconstruction of attosecond beating by interference of two-photon transitions) method. The key idea involves the comparison of two measurements with different orders of CC transitions. The scheme is illustrated by an ab initio calculation on atomic hydrogen.
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.
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.