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Two-photon resonant excitation of a doubly excited state in He atoms by high-harmonic pulses

Taro Sekikawa, Tatsuya Okamoto, Eisuke Haraguchi, Mikio Yamashita, Takashi Nakajima

Published Dec 17, 2008• 25 citations
Publisher

Abstract

We experimentally demonstrate a two-color two-photon resonant excitation of the doubly excited 2p2 1S state in helium atoms by the combination of 19th and 21st harmonic photons of a Ti:sapphire laser. Production of the 2p2 1S state is confirmed by the experimental observation that the electron emission from this state does not depend on the direction of harmonic polarization. Our ab-initio theoretical results through the solution of time-dependent Schrödinger equation are consistent with the experimental results and confirm the first successful production of a doubly excited state by high-harmonic pulses.

DOI
10.1364/oe.16.021922

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We experimentally demonstrate a two-color two-photon resonant excitation of the doubly excited 2p2 1S state in helium atoms by the combination of 19th and 21st harmonic photons of a Ti:sapphire laser. Production of the 2p2 1S state is confirmed by the experimental observation that the electron emission from this state does not depend on the direction of harmonic polarization. Our ab-initio theoretical results through the solution of time-dependent Schrödinger equation are consistent with the experimental results and confirm the first successful production of a doubly excited state by high-harmonic pulses.
We study resonant two-color two-photon ionization of helium via the 1s3p (1)P(1) state. The first color is the 15th harmonic of a tunable Ti:sapphire laser, while the second color is the fundamental laser radiation. Our method uses phase-locked high-order harmonics to determine the phase of the two-photon process by interferometry. The measurement of the two-photon ionization phase variation as a function of detuning from the resonance and intensity of the dressing field allows us to determine the intensity dependence of the transition energy.
We discuss the dynamics of the two-photon resonant ionization of helium involving two autoionizing states in the presence of two-color laser fields. The first source is tuned around the transition from the ground state to the 2s2p 1Po autoionizing state, and the second couples the state 2s2p 1Po to the 2p2 1S autoionizing state. The laser coupling between the doubly excited states is shown to lead to modifications of the Beutler-Fano profile and the appearance of an Autler-Townes doublet. This double resonance effect between autoionizing states can be observed at moderate laser intensities easily attainable by currently operated sources.
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.
We present experimental results and theoretical analysis of two-photon ionization of He by a superposition of the 7th to the 13th harmonic of a Ti:sapphire laser. Solving the time-dependent Schrödinger equation for He in a coherent polychromatic field, the He+ yield is calculated. From this yield the number of He+ ions produced has been estimated and found in reasonable agreement with its measured value. The present results establish the feasibility of a second-order autocorrelation measurement of superposition of harmonics, and thus they represent the precursor towards the direct temporal characterization of attosecond pulse trains.
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 time-dependent Schr\"odinger equation for the helium atom with a model potential is solved on a numerical grid. The effects of intermediate-state resonance and of the ionization of the atom upon the harmonic generation are investigated. We also evaluate the contribution of the helium ion when the laser intensity is sufficiently high for most of the atoms to be ionized during the laser pulse. We find that the harmonics with order higher than 13 are due to the ion when the photon energy is 5.0 eV, while for photon energy 2.0 eV the atom produces up to about the 49th harmonic.