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arXiv:1211.2566

Attosecond Transient Absorption Spectroscopy of doubly-excited states in helium

Luca Argenti, Christian Ott, Thomas Pfeifer, Fernando Martı́n

Published Nov 12, 2012• 2 citations
arXivHTMLPDF

Abstract

Strong-field manipulation of autoionizing states is a crucial aspect of electronic quantum control. Recent measurements of the attosecond transient absorption spectrum of helium dressed by a few-cycle visible pulse [Ott et al., arXiv:1205.0519[physics.atom-ph] ] provide evidence of novel ultrafast resonant phenomena, namely, two-photon Rabi oscillations between doubly-excited states and the inversion of Fano profiles. Here we present the results of accurate \emph{ab-initio} calculations that agree with these observations and in addition predict that (i) inversion of Fano profiles is actually periodic in the coupling laser intensity and (ii) the supposedly dark $2p^2$ {$^1$S} state also appears in the spectrum. Closer inspection of the experimental data confirms the latter prediction.

DOI
10.48550/arxiv.1211.2566

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Strong-field manipulation of autoionizing states is a crucial aspect of electronic quantum control. Recent measurements of the attosecond transient absorption spectrum of helium dressed by a few-cycle visible pulse [Ott et al., arXiv:1205.0519[physics.atom-ph] ] provide evidence of novel ultrafast resonant phenomena, namely, two-photon Rabi oscillations between doubly-excited states and the inversion of Fano profiles. Here we present the results of accurate \emph{ab-initio} calculations that agree with these observations and in addition predict that (i) inversion of Fano profiles is actually periodic in the coupling laser intensity and (ii) the supposedly dark 2p22p^22p2 {1^11S} state also appears in the spectrum. Closer inspection of the experimental data confirms the latter prediction.
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.
In the present paper, we investigate the time-resolved transient absorption spectroscopy of doubly excited states of helium atoms by solving the time-dependent two-electron Schr\"odinger equation numerically based on a one-dimensional model. The helium atoms are subjected to an extreme ultraviolet (XUV) attosecond pulse and a time-delayed infrared (IR) few-cycle laser pulse. A superposition of doubly excited states populated by the XUV pulse is identified, which interferes with the direct ionization pathway leading to Fano resonance profiles in the photoabsorption spectrum. In the presence of an IR laser, however, the Fano line profiles are strongly modified: A shifting, splitting, and broadening of the original absorption lines is observed when the XUV attosecond pulse and infrared few-cycle laser pulse overlap in time, which is in good agreement with recent experimental results. At certain time delays, we observe symmetric Lorentz, inverted Fano profiles, and even negative absorption cross sections indicating that the XUV light can be amplified during the interaction with atoms. We further prove that the above pictures are general for different doubly excited states by suitably varying the frequency of the IR field to coherently couple the corresponding states.
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.
The helium atom, with one nucleus and two electrons, is a prototypical system to study quantum many-body dynamics. Doubly excited states, or quantum states in which both electrons are excited by one photon, showcase electronic-correlation mediated effects. In this paper, the natural lifetimes of the doubly excited 1 P o 2 s n p Rydberg series and the 1 S e 2 p 2 dark state in helium in the 60–65 eV region are measured directly in the time domain with extreme-ultraviolet/near-infrared noncollinear attosecond four-wave-mixing (FWM) spectroscopy. The measured lifetimes agree with lifetimes deduced from spectral linewidths and theoretical predictions, and the roles of specific decay mechanisms are considered. While complex spectral line shapes in the form of Fano resonances are common in absorption spectroscopy of autoionizing states, the background-free and thus homodyned character of noncollinear FWM results exclusively in Lorentzian spectral features in the absence of strong-field effects. The onset of strong-field effects that would affect the extraction of accurate natural lifetimes in helium by FWM is determined to be approximately 0.3 Rabi cycles. This study provides a systematic understanding of the FWM parameters necessary to enable accurate lifetime extractions, which can be utilized in more complex quantum systems in the future. Published by the American Physical Society 2024
We present theoretical simulations of the attosecond transient absorption of singly-excited states of helium atoms in the presence of a dressing near-infrared or infrared laser. In particular, we aim to address several unresolved questions in the transient absorption of helium and to resolve the remaining discrepancies between theory and experiment. We initially focus on the forklike structures in the Autler–Townes splitting of the 1s2p state and the effects of resonant coupling to the 1s2s and 1s3s states. We find that the delay-dependent features of the Autler–Townes doublet depend strongly on both the laser frequency detuning from resonance and on the laser pulse duration, and explain the lack of such structures in current experimental data. Next, we identify the interference mechanism which causes the half-cycle oscillations in the absorption spectrum below the excited state manifold. Finally, we observe for the first time the presence of quantum beating in the simulated transient absorption spectrogram, and discuss the conditions under which such wavepacket dynamics could be observed experimentally.