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arXiv:1907.06874 · Physical Review Letters

Strong-Field Extreme-Ultraviolet Dressing of Atomic Double Excitation

Christian Ott, Lennart Aufleger, Thomas Ding, Marc Rebholz, Alexander Magunia, Maximilian Hartmann, Veit Stooß, David Wachs, Paul Birk, Gergana Dimitrova Borisova, Kristina Meyer, Patrick Rupprecht, Carina da Costa Castanheira, R. Moshammer, Andrew Attar, Thomas Gaumnitz, Zhi-Heng Loh, S. Düsterer, R. Treusch, J. Ullrich, Yuhai Jiang, Michael Meyer, P. Lambropoulos, Thomas Pfeifer

Published Oct 15, 2019• 51 citations
arXivHTMLPDF

Abstract

We report on the experimental observation of a strong-field dressing of an autoionizing two-electron state in helium with intense extreme-ultraviolet laser pulses from a free-electron laser. The asymmetric Fano line shape of this transition is spectrally resolved, and we observe modifications of the resonance asymmetry structure for increasing free-electron-laser pulse energy on the order of few tens of Microjoules. A quantum-mechanical calculation of the time-dependent dipole response of this autoionizing state, driven by classical extreme-ultraviolet (XUV) electric fields, evidences strong-field-induced energy and phase shifts of the doubly excited state, which are extracted from the Fano line-shape asymmetry. The experimental results obtained at the Free-Electron Laser in Hamburg (FLASH) thus correspond to transient energy shifts on the order of a few meV, induced by strong XUV fields. These results open up a new way of performing nonperturbative XUV nonlinear optics for the light-matter interaction of resonant electronic transitions in atoms at short wavelengths.

DOI
10.1103/physrevlett.123.163201

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We report on the experimental observation of a strong-field dressing of an autoionizing two-electron state in helium with intense extreme-ultraviolet laser pulses from a free-electron laser. The asymmetric Fano line shape of this transition is spectrally resolved, and we observe modifications of the resonance asymmetry structure for increasing free-electron-laser pulse energy on the order of few tens of Microjoules. A quantum-mechanical calculation of the time-dependent dipole response of this autoionizing state, driven by classical extreme-ultraviolet (XUV) electric fields, evidences strong-field-induced energy and phase shifts of the doubly excited state, which are extracted from the Fano line-shape asymmetry. The experimental results obtained at the Free-Electron Laser in Hamburg (FLASH) thus correspond to transient energy shifts on the order of a few meV, induced by strong XUV fields. These results open up a new way of performing nonperturbative XUV nonlinear optics for the light-matter interaction of resonant electronic transitions in atoms at short wavelengths.
We report on numerical results revealing line-shape asymmetry changes of electronic transitions in atoms near-resonantly driven by intense extreme-ultraviolet (XUV) electric fields by monitoring their transient absorption spectrum after transmission through a moderately dense atomic medium. Our numerical model utilizes ultrashort broadband XUV laser pulses varied in their intensity (1014–1015 W/cm2) and detuning nearly out of resonance for a quantitative evaluation of the absorption line-shape asymmetry. It will be shown how transient energy shifts of the bound electronic states can be linked to these asymmetry changes in the case of an ultrashort XUV driving pulse temporally shorter than the lifetime of the resonant excitation, and how the asymmetry can be controlled by the near-resonant detuning of the XUV pulse. In the case of a two-level system, the numerical model is compared to an analytical calculation, which helps to uncover the underlying mechanism for the detuning- and intensity-induced line-shape modification and links it to the generalized Rabi frequency. To further apply the numerical model to recent experimental results of the near-resonant dressing of the 2s2p doubly excited state in helium by an ultrashort XUV free-electron laser pulse we extend the two-level model with an ionization continuum, thereby enabling the description of transmission-type (Fraunhofer-like) transient absorption of a strongly laser-coupled autoionizing state.
Within this work, electron dynamics of autoionizing, doubly excited states in helium are investigated. Therefore, strong field couplings of these states are studied in two spectral regimes: in the infrared and in the extreme ultraviolet. A laser system capable of tuning its output-pulses' central wavelength within the infrared spectral regime is installed and characterized by a FROG setup. Furthermore, high harmonics of these output pulses are generated and discussed. First intensity dependent and time resolved experiments in helium with this laser system are presented and supported by numerical calculations. The transition from an unperturbed light induced state, which is generated from the 2p4p state, to a resonant Autler-Townes splitting of the sp2;3+ state is observed. Furthermore, strong field couplings between the ground and a doubly-excited state are studied in the extreme ultraviolet only regime. With the help of simulations Rabi-like couplings and Stark shifts for ultrashort pulses leading to a manipulated absorption line shape are investigated. The same study is carried out for autoionizing states. This theory part is used to explain experimentally measured line-shape changes of the 2s2p resonance in helium interacting with FEL pulses.
The coherent excitation and manipulation of a two-level system with ultrashort intense extreme-ultraviolet laser fields is investigated theoretically, based on numerically solving the time-dependent Schr\"odinger equation. We are particularly interested in the dynamical phase excursion of the energy states over the course of the interaction and the resulting spectral modifications. Fitting the absorption line shapes with the Fano profile quantifies the asymmetry parameter and the corresponding dipole phase offset, capturing the phase difference of the state coefficients after the interaction. Nonperturbative analytical calculations using rectangular driving pulses are employed, yielding physical insights into the dependence of the dipole phase shift on the external field. The validity of the formulas is validated by comparing their predictions with numerical results, which proves to be robust against the variation of laser parameters. The present investigation of strong-field dressing effects complements recent attosecond transient absorption studies assuming weak excitation, and marks a ubiquitous phenomenon that should be generally considered for the interaction of matter with intense laser fields.
We report time-resolved photoelectron spectroscopy of the 3s3p3s3p3s3p doubly excited states of helium dressed by an intense near-infrared (NIR) laser field. Using synchronized XUV free-electron-laser and 800-nm NIR laser pulses, we observe a pronounced delay-dependent shift of resonance-related spectral minima together with the emergence of additional structures around the NIR sideband energy. \textit{Ab initio} theoretical calculations support these observations and identify the features as signatures of NIR-induced coupling of the bright (3s3p1Po3s3p {}^{1}P^{o}3s3p1Po) autoionizing state to nearby dark (1De^{1}D^{e}1De and 1Se^{1}S^{e}1Se) resonances below the N=3N = 3N=3 threshold. A multichannel Fano resonance analysis of the measured spectra yields delay-dependent line-shape parameters and resonance energies, establishing a quantitative route to characterize and control correlated two-electron resonances in strong laser fields.
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.
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.