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arXiv:1205.4775 · Physical Review A

Laser-assisted-autoionization dynamics of helium resonances with single attosecond pulses

Wei-Chun Chu, Song-Feng Zhao, C. D. Lin

Published Sep 29, 2011• 40 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physreva.84.033426

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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(1P)2s2p{(}^{1}\phantom{\rule{0.16em}{0ex}}P)2s2p(1P) resonance state in the presence of an intense infrared (IR) laser. The laser field introduces strong coupling between 2s2p(1P)2s2p{(}^{1}\phantom{\rule{0.16em}{0ex}}P)2s2p(1P) and 2p2(1S)2{p}^{2}{(}^{1}\phantom{\rule{0.16em}{0ex}}S)2p2(1S) 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(1P)2s2p{(}^{1}\phantom{\rule{0.16em}{0ex}}P)2s2p(1P) and 2s2(1S)2{s}^{2}{(}^{1}\phantom{\rule{0.16em}{0ex}}S)2s2(1S) by examining how the photoelectron spectra are modified versus the time delay and the possibility of observing Autler-Townes doublet in such experiments.
We study theoretically the photoabsorption spectra of an attosecond extreme ultraviolet (XUV) pulse by a laser-dressed atomic system. A weak XUV excites an autoionizing state which is strongly coupled to another autoionizing state by a laser. The theory was applied to explain two recent experiments [Loh, Greene, and Leone, Chem. Phys. 350, 7 (2008); Wang, Chini, Chen, Zhang, Cheng, He, Cheng, Wu, Thumm, and Chang, Phys. Rev. Lett. 105, 143002 (2010)] where the absorption spectra of the XUV lights were measured against the time delay between the laser and the XUV. In another example, we study an attosecond pulse exciting the 2s2p(1P)2s2p{(}^{1}\phantom{\rule{-0.16em}{0ex}}P)2s2p(1P) resonance of helium which is resonantly coupled to the 2s2(1S)2{s}^{2}{(}^{1}\phantom{\rule{-0.16em}{0ex}}S)2s2(1S) resonance by a moderately intense 540-nm laser. The relation between the photoabsorption spectra and the photoelectron spectra and the modification of the transmitted lights in such an experiment are analyzed. The role of Rabi flopping between the two autoionizing states within their lifetimes is investigated with respect to the laser intensity and detuning.
We discuss the dynamics of doubly resonant ionization in helium involving the strong coupling of two doubly excited autoionizing resonances, under the influence of XUV radiation of short duration (DESY FEL) and a synchronized optical laser. We explore the possibility of using the photoelectron spectra to extract information about the pulse shape of the FEL. We present in addition new calculations of the expected AC Stark splitting due to the strong coupling of the two resonances and show that, within the range of intensities and pulse durations expected in the experiments, additional structure, beyond the usual doublet, is to be expected.
We study the photoelectron spectra of hydrogen and helium ionized by intense ultrafast two-color XUV laser pulses by numerically solving the time-dependent Schrödinger equation.The photon energy of the pump pulse is tuned to the 1s-2p excitation energy, inducing Rabi oscillations between these bound states and forming an Autler-Townes (AT) doublet of dressed states.When ionized by a time-delayed ultrafast XUV pulse with duration shorter than the Rabi oscillation period, we find novel and drastically enhanced AT splittings in the photoionization spectrum.We identify their origin in terms of the temporal interference of two attosecond wave packets whose spectral distribution is controlled by the interplay between Rabi frequency and bandwidth of the probe pulse.These time-dependent features in the spectra can be much larger than the standard AT spacing induced by the pump pulse alone and can be controlled by the time delay and the duration of the probe pulse.
Helium atoms in the presence of extreme ultraviolet light pulses can lose electrons through direct photoionization or through two-electron excitation followed by autoionization. Here we demonstrate that, by combining attosecond extreme ultraviolet pulses with near infrared femtosecond lasers, electron dynamics in helium autoionization can be not only monitored but also controlled. Furthermore, the interference between the two ionization channels was modified by the intense near infrared laser pulse. To the best of our knowledge, this is the first time that double excitation and autoionization were studied experimentally by using isolated attosecond pulses.
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.
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.