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Optics Express

Quantitative uncertainty determination of phase retrieval in RABBITT

Jia-Bao Ji, Saijoscha Heck, Meng Han, Hans Jakob Wörner

Published Jul 22, 2021• 7 citations
Publisher

Abstract

Reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) is one of the most widely used approaches to measure the time delays in photoionization. The time delay, which corresponds to a phase difference of two oscillating signals, is usually retrieved by cosine fitting or fast Fourier transform (FFT). We propose two estimators for the phase uncertainty of cosine fitting from the signal per se of an individual experiment: (i) σ ( φ fit ) ≈ B A 2 N , where B/A is the mean-value-to-amplitude ratio, and N is the total count number, and (ii) σ ( φ fit ) ≈ 1 − R 2 R 2 n bins , where nbins is the total number of bins in the time domain, and R2 is the coefficient of determination. The former estimator is applicable for the statistical fluctuation, while the latter includes the effects from various uncertainty sources, which is mathematically proven and numerically validated. This leads to an efficient and reliable approach to determining quantitative uncertainties in RABBITT experiments and evaluating the observed discrepancy among individual measurements, as demonstrated on the basis of experimental data.

DOI
10.1364/oe.432222

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Reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) is one of the most widely used approaches to measure the time delays in photoionization. The time delay, which corresponds to a phase difference of two oscillating signals, is usually retrieved by cosine fitting or fast Fourier transform (FFT). We propose two estimators for the phase uncertainty of cosine fitting from the signal per se of an individual experiment: (i) σ ( φ fit ) ≈ B A 2 N , where B/A is the mean-value-to-amplitude ratio, and N is the total count number, and (ii) σ ( φ fit ) ≈ 1 − R 2 R 2 n bins , where nbins is the total number of bins in the time domain, and R2 is the coefficient of determination. The former estimator is applicable for the statistical fluctuation, while the latter includes the effects from various uncertainty sources, which is mathematically proven and numerically validated. This leads to an efficient and reliable approach to determining quantitative uncertainties in RABBITT experiments and evaluating the observed discrepancy among individual measurements, as demonstrated on the basis of experimental data.
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.
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
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.
Reconstruction of attosecond beating by interference of two-photon transitions is a cornerstone technique of attosecond chronoscopy, routinely used to extract photoemission delays from the phase of sideband oscillations. Here, we theoretically investigate the reconstruction of attosecond beating by interference of two-photon transitions protocol driven by quantum light and demonstrate that it is intrinsically sensitive to the quantum nature of the driving field. When the probe field is prepared in a nonclassical state, its photon statistics are imprinted onto photoelectrons via continuum-continuum transitions, giving rise to an additional time delay of several tens of attoseconds. We trace this delay to the phase associated with the second-order anomalous moment ⟨a[over ^]^{2}⟩ of the probe field. Extending the framework to a three-sideband configuration, which enables retrieval of the fourth-order anomalous moment ⟨a[over ^]^{4}⟩, we show that the interferometer exhibits significantly enhanced sensitivity to quantum fluctuations. Our work illustrates quantum attosecond photoelectron interferometry as a phase-sensitive probe of quantum light, offering a promising route for time-resolved quantum metrology at the attosecond scale.
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.