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Optics Young Scientist Summit (OYSS)

Coherent control of photon-dressed fringes by attosecond transient absorption

Qianyu Qiu, Guangru Bai, Qian Zhang, Zengxiu Zhao

Published Dec 29, 2023• 0 citations
Publisher

Abstract

Line shapes observed in attosecond transient absorption spectra (ATAS) encode information on the phase of the optical dipole response. Understanding and controlling the phase evolution of interference fringes is among the fundamental goals of exploring coherent interaction. Here, we simulate the attosecond transient absorption in the near-infrared (NIR) dressing field by considering a three-level model in the adiabatic approximation. We find that the absorption line shape can be changed from Lorentzian to Fano to inverted Lorentzian and back again at two-photon dressed energy levels “ω ± 2ωι”, and line shapes evolve in half-cycle periodicity (T/2). Moreover, the direction of phase evolution of “ω ± 2ωι” is opposite, while the phases of “ω ± 2ωι” are roughly the same at certain delays with an interval of approximately a quarter-cycle periodicity (T/4). These results demonstrate that absorbance of two-photon dressed energy levels “ω ± 2ωι” can qualitatively map the AC Stark shift. These observations provide new insights into the control of spectral line shapes and open the way for the modulation of quantum optical interference in the laser-driven atom.

DOI
10.1117/12.3015142

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Line shapes observed in attosecond transient absorption spectra (ATAS) encode information on the phase of the optical dipole response. Understanding and controlling the phase evolution of interference fringes is among the fundamental goals of exploring coherent interaction. Here, we simulate the attosecond transient absorption in the near-infrared (NIR) dressing field by considering a three-level model in the adiabatic approximation. We find that the absorption line shape can be changed from Lorentzian to Fano to inverted Lorentzian and back again at two-photon dressed energy levels “ω ± 2ωι”, and line shapes evolve in half-cycle periodicity (T/2). Moreover, the direction of phase evolution of “ω ± 2ωι” is opposite, while the phases of “ω ± 2ωι” are roughly the same at certain delays with an interval of approximately a quarter-cycle periodicity (T/4). These results demonstrate that absorbance of two-photon dressed energy levels “ω ± 2ωι” can qualitatively map the AC Stark shift. These observations provide new insights into the control of spectral line shapes and open the way for the modulation of quantum optical interference in the laser-driven atom.
We simulate the transient absorption of attosecond pulses of infrared-laser-dressed atoms by considering a three-level system in the adiabatic approximation. The delay-dependent interference features are investigated from the perspective of the coherent interaction processes between the attosecond pulse and the quasiharmonics. We find that many features of the interference fringes in the absorption spectra of the attosecond pulse can be attributed to the coherence phase difference. However, the modulation signals of laser-induced sidebands of the dark state are found to be related to the population dynamics of the dark state by the dressing field.
The attosecond pump-femtosecond probe technique is widely used in electron dynamics research, with temporal resolution reaching tens of attoseconds. Here, we propose a scheme for controlling the Fano line shapes of helium doubly excited states by replacing the pump source with a pair of time-delayed attosecond pulses. We show that the interference induced by this delay provides an additional, highly effective means of controlling electron dynamics, enabling temporal resolution on the zeptosecond scale. We demonstrate that the corresponding line shapes in transient absorption spectra can shift dramatically within a time-delay variation of just a few hundred zeptoseconds. This extreme spectral modulation occurs under two key conditions: (i) when the time delay aligns with the spectral minimum of the coherently combined attosecond pulses in the frequency domain, and (ii) when the delay between the infrared probe pulse and the first attosecond pulse is held constant. This approach opens a new pathway to zeptosecond-scale control in quantum systems and demonstrates the powerful synergy between phase manipulation in both light and electron waves for achieving ultrafast spectral transformations.
Strong-field manipulation of autoionizing states is a crucial aspect of electronic quantum control. Recent measurements of the attosecond transient absorption spectrum (ATAS) of helium dressed by a few-cycle visible pulse [C. Ott et al , Nature 516, 374 (2014)] provide evidence of the inversion of Fano profiles. With the support of accurate ab-initio calculations that reproduce the results of the latter experiment, here we investigate the new physics that arise from ATAS when the laser intensity is increased. In particular, we show that (i) previously unnoticed signatures of the dark 2 p 2 1 S doubly excited state are observed in the experimental spectrum, (ii) inversion of Fano profiles is predicted to be periodic in the laser intensity, and (iii) the ac-Stark shift of the higher terms in the sp + 2, n autoionizing series exceeds the ponderomotive energy, which is the result of a genuine two-electron contribution to the polarization of the excited atom.
Strong-field manipulation of autoionizing states is a crucial aspect of electronic quantum control. Recent measurements of the attosecond transient absorption spectrum (ATAS) of helium dressed by a few-cycle visible pulse [C. Ott et al., Nature (London) 516, 374 (2014)] provide evidence of the inversion of Fano profiles. With the support of accurate ab initio calculations that reproduce the results of the latter experiment, here we investigate the new physics that arise from ATAS when the laser intensity is increased. In particular, we show that (i) previously unnoticed signatures of the dark 2p21S2{p}^{2}{\phantom{\rule{0.16em}{0ex}}}^{1}S2p21S doubly excited state are observed in the experimental spectrum, (ii) inversion of Fano profiles is predicted to be periodic in the laser intensity, and (iii) the ac Stark shift of the higher terms in the sp2,n+s{p}_{2,n}^{+}sp2,n+​ autoionizing series exceeds the ponderomotive energy, which is the result of a genuine two-electron contribution to the polarization of the excited atom.
We investigate the evolution of extreme ultraviolet (XUV) spectral line shapes in an optically thick helium gas under near-infrared (IR) perturbation. In our experimental and theoretical work, we systematically vary the IR intensity, time-delay, gas density, and IR polarization parameters to study line-shape modifications induced by collective interactions in a regime beyond the single-atom response of a thin, dilute gas. In both experiment and theory, we find that specific features in the frequency-domain absorption profile, and their evolution with propagation distance, can be attributed to the interplay between resonant attosecond pulse propagation and IR-induced phase shifts. Our calculations show that this interplay also manifests itself in the time domain, with the IR pulse influencing the reshaping of the XUV pulse propagating in the resonant medium.
We calculate the transient absorption of an isolated attosecond pulse (IAP) by helium atoms subject to a delayed infrared (IR) laser pulse. With the central frequency of the broad attosecond spectrum near the ionization threshold, the absorption spectrum is strongly modulated at the sub-IR-cycle level. Given that the absorption spectrum results from a time-integrated measurement, we investigate the extent to which the delay dependence of the absorption yields information about the attosecond dynamics of the atom-field energy exchange. We find two configurations in which this is possible. The first involves multiphoton transitions between bound states that result in interference between different excitation pathways. The second involves the modification of the bound state absorption lines by the IR field, which we find can result in a subcycle time dependence only when ionization limits the duration of the strong-field interaction.