Physical Review Letters

Attosecond Time-Resolved Autoionization of Argon

He Wang, Michael Chini, Shouyuan Chen, C.-H. Zhang, Feng He, Yan Cheng, Yi Wu, Uwe Thumm, Zenghu Chang

Published Oct 1, 2010• 376 citations

Abstract

Autoionization of argon atoms was studied experimentally by transient absorption spectroscopy with isolated attosecond pulses. The peak position, intensity, linewidth, and shape of the 3s3p⁶np ¹P Fano resonance series (26.6-29.2 eV) were modified by intense few-cycle near infrared laser pulses, while the delay between the attosecond pulse and the laser pulse was changed by a few femtoseconds. Numerical simulations revealed that the experimentally observed splitting of the 3s3p⁶4p ¹P line is caused by the coupling between two short-lived highly excited states in the strong laser field.

DOI: 10.1103/physrevlett.105.143002

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Physical Review Letters

Attosecond Time-Resolved Autoionization of Argon

He Wang, Michael Chini, Shouyuan Chen, C.-H. Zhang, Feng He, Yan Cheng, Yi Wu, Uwe Thumm, Zenghu Chang

Published Oct 1, 2010• 376 citations

Publisher

Abstract

DOI: 10.1103/physrevlett.105.143002

Related papers

Experimental observation of ultrashort laser pulse effects on the autoionization dynamics of argon atoms

Arso Ivanovic

Within this work, electron dynamics inside argon atoms are observed by probing the autoionizing states of argon atoms, so-called window resonances, with both attosecond XUV and timed-delayed few-cycle femtosecond NIR laser pulses, using attosecond transient absorption spectroscopy. The window resonances in the energy region of 25 - 29.3 eV are first excited with the XUV pulse and then dressed by the NIR laser, where the natural decay process of the states is greatly affected by the strong-field of the NIR pulse. Preliminary results of the measurement are presented in this work, with a hypothetical description of some of the effects that are present. A comparison has been made with the experimental results from a paper publishing measurements of autoionizing states with attosecond transient absorption spectroscopy for the first time, where the same resonances were probed. The comparison is only partly possible due to different experimental parameters and conditions, where more pronounced and new effects have been observed in the here performed measurement.Within this work, electron dynamics inside argon atoms are observed by probing the autoionizing states of argon atoms, so-called window resonances, with both attosecond XUV and timed-delayed few-cycle femtosecond NIR laser pulses, using attosecond transient absorption spectroscopy. The window resonances in the energy region of 25 - 29.3 eV are first excited with the XUV pulse and then dressed by the NIR laser, where the natural decay process of the states is greatly affected by the strong-field of the NIR pulse. Preliminary results of the measurement are presented in this work, with a hypothetical description of some of the effects that are present. A comparison has been made with the experimental results from a paper publishing measurements of autoionizing states with attosecond transient absorption spectroscopy for the first time, where the same resonances were probed. The comparison is only partly possible due to different experimental parameters and conditions, where more pronounced and new effects have been observed in the here performed measurement.

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Watching the formation and reshaping of a Fano resonance in a macroscopic medium

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Time-resolved buildup of a Fano resonance in a macroscopic gaseous medium is theoretically studied by attosecond transient absorption spectroscopy. An intense near-infrared field is employed as an adjustable gate to confine the temporal dynamics, enabling one to resolve the line-shape formation in real time. Beyond the region where the single-atom approximation holds, we observe the emergence of spectral spikes with narrow linewidths for certain time delays and propagation distances, which represents that the medium can be delicately structured to be an efficient resonant absorber. Spectral substructures appear on the shoulder of the absorption lines after additional pulse propagation. The links between these features imprinted in spectral profiles and the formation of temporal characteristics in the excitation field are identified. The collective response of the medium versus time delay and propagation distance, in this laser-gated case, provides clues to the time-domain information on autoionization state and the microscopic dynamics occurring at each layer of the medium.Time-resolved buildup of a Fano resonance in a macroscopic gaseous medium is theoretically studied by attosecond transient absorption spectroscopy. An intense near-infrared field is employed as an adjustable gate to confine the temporal dynamics, enabling one to resolve the line-shape formation in real time. Beyond the region where the single-atom approximation holds, we observe the emergence of spectral spikes with narrow linewidths for certain time delays and propagation distances, which represents that the medium can be delicately structured to be an efficient resonant absorber. Spectral substructures appear on the shoulder of the absorption lines after additional pulse propagation. The links between these features imprinted in spectral profiles and the formation of temporal characteristics in the excitation field are identified. The collective response of the medium versus time delay and propagation distance, in this laser-gated case, provides clues to the time-domain information on autoionization state and the microscopic dynamics occurring at each layer of the medium.

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Luca Argenti, Christian Ott, Thomas Pfeifer +1 more

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.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.

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Absorption and emission of single attosecond light pulses in an autoionizing gaseous medium dressed by a time-delayed control field

Wei-Chun Chu, C. D. Lin

An extreme ultraviolet (EUV) single attosecond pulse passing through a laser-dressed dense gas is studied theoretically. The weak EUV pulse pumps the helium gas from the ground state to the $2s2p({}^{1}P)$ autoionizing state, which is coupled to the $2{s}^{2}{(}^{1}S)$ autoionizing state by a femtosecond infrared laser with the intensity in the order of 10 ${}^{12}$ W/cm ${}^{2}$ . The simulation shows how the transient absorption and emission of the EUV are modified by the coupling laser. A simple analytical expression for the atomic response derived for $\ensuremath{\delta}$-function pulses reveals the strong modification of the Fano lineshape in the spectra, where these features are quite universal and remain valid for realistic pulse conditions. We further account for the propagation of pulses in the medium and show that the EUV signal at the atomic resonance can be enhanced in the gaseous medium by more than 50 $%$ for specifically adjusted laser parameters, and that this enhancement persists as the EUV propagates in the gaseous medium. Our result demonstrates the high-level control of nonlinear optical effects that are achievable with attosecond pulses.An extreme ultraviolet (EUV) single attosecond pulse passing through a laser-dressed dense gas is studied theoretically. The weak EUV pulse pumps the helium gas from the ground state to the $2s2p({}^{1}P)$ autoionizing state, which is coupled to the $2{s}^{2}{(}^{1}S)$ autoionizing state by a femtosecond infrared laser with the intensity in the order of 10${}^{12}$ W/cm${}^{2}$. The simulation shows how the transient absorption and emission of the EUV are modified by the coupling laser. A simple analytical expression for the atomic response derived for $\ensuremath{\delta}$-function pulses reveals the strong modification of the Fano lineshape in the spectra, where these features are quite universal and remain valid for realistic pulse conditions. We further account for the propagation of pulses in the medium and show that the EUV signal at the atomic resonance can be enhanced in the gaseous medium by more than 50$%$ for specifically adjusted laser parameters, and that this enhancement persists as the EUV propagates in the gaseous medium. Our result demonstrates the high-level control of nonlinear optical effects that are achievable with attosecond pulses.

arXiv:1211.6172Physical Review AJan 16, 201345 citations

The strong coupling between two autoionizing states in helium is studied theoretically with the pump-probe scheme. An isolated 100-as XUV pulse is used to excite helium near the

2s2p{(}^{1}\phantom{\rule{0.16em}{0ex}}P)

resonance state in the presence of an intense infrared (IR) laser. The laser field introduces strong coupling between

2s2p{(}^{1}\phantom{\rule{0.16em}{0ex}}P)

and

2{p}^{2}{(}^{1}\phantom{\rule{0.16em}{0ex}}S)

states. The IR also can ionize helium from both autoionizing states. By changing the time delay between the XUV and the IR pulses, we investigated the photoelectron spectra near the two resonances. The results are used to explain the recent experiment by Gilbertson et al. [Phys. Rev. Lett. 105, 263003 (2010)]. Using the same isolated attosecond pulse and a 540-nm laser, we also investigate the strong coupling between

2s2p{(}^{1}\phantom{\rule{0.16em}{0ex}}P)

and

2{s}^{2}{(}^{1}\phantom{\rule{0.16em}{0ex}}S)

by examining how the photoelectron spectra are modified versus the time delay and the possibility of observing Autler-Townes doublet in such experiments.

2p^2

{

^1

S} state also appears in the spectrum. Closer inspection of the experimental data confirms the latter prediction.

An extreme ultraviolet (EUV) single attosecond pulse passing through a laser-dressed dense gas is studied theoretically. The weak EUV pulse pumps the helium gas from the ground state to the

2s2p({}^{1}P)

autoionizing state, which is coupled to the

2{s}^{2}{(}^{1}S)

autoionizing state by a femtosecond infrared laser with the intensity in the order of 10

{}^{12}

W/cm

{}^{2}

. The simulation shows how the transient absorption and emission of the EUV are modified by the coupling laser. A simple analytical expression for the atomic response derived for $\ensuremath{\delta}$-function pulses reveals the strong modification of the Fano lineshape in the spectra, where these features are quite universal and remain valid for realistic pulse conditions. We further account for the propagation of pulses in the medium and show that the EUV signal at the atomic resonance can be enhanced in the gaseous medium by more than 50

%

for specifically adjusted laser parameters, and that this enhancement persists as the EUV propagates in the gaseous medium. Our result demonstrates the high-level control of nonlinear optical effects that are achievable with attosecond pulses.