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Physical Review A

Effects of coherent coupling of autoionizing states on multiphoton ionization

Natalia E. Karapanagioti, Dimitrios Charalambidis, Cornelis J. G. J. Uiterwaal, Costas Fotakis, H. Bachau, I. Sánchez, E. Cormier

Published Apr 1, 1996• 59 citations
Publisher

Abstract

We present the experimental and theoretical investigation of the effects of the strong electromagnetic coupling of two autoionizing states (AIS's) on the photoionization properties of an atomic system. These effects are observed by probing the ladder system from the ground state of the atom through a weak two-photon transition to the region of the lower AIS. The experimental observation of the modification of the total ionization and partial photoelectron spectra at different wavelengths of the coupling and probe lasers are accurately reproduced by a theoretical analysis which uses a density-matrix approach. Both theory and experiment indicate a strong inhibition of the ionization of the system in the case when both lasers are resonant with the two atomic transitions, while displaying a rapidly varying asymmetry induced as the detuning between the two states and the fields increases. In the extreme case of a large detuning, two separate structures appear as distinct total ionization and photoelectron peaks. The above findings combined with the full theoretical treatment indicate that the phenomena observed are an experimental demonstration of ac Stark splitting between two AIS's. \textcopyright{} 1996 The American Physical Society.

DOI
10.1103/physreva.53.2587

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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Oct 21, 1998•0 citations
We present the experimental and theoretical investigation of the effects of the strong electromagnetic coupling of two autoionizing states (AIS's) on the photoionization properties of an atomic system. These effects are observed by probing the ladder system from the ground state of the atom through a weak two-photon transition to the region of the lower AIS. The experimental observation of the modification of the total ionization and partial photoelectron spectra at different wavelengths of the coupling and probe lasers are accurately reproduced by a theoretical analysis which uses a density-matrix approach. Both theory and experiment indicate a strong inhibition of the ionization of the system in the case when both lasers are resonant with the two atomic transitions, while displaying a rapidly varying asymmetry induced as the detuning between the two states and the fields increases. In the extreme case of a large detuning, two separate structures appear as distinct total ionization and photoelectron peaks. The above findings combined with the full theoretical treatment indicate that the phenomena observed are an experimental demonstration of ac Stark splitting between two AIS's. \textcopyright{} 1996 The American Physical Society.
The coherent resonant coupling of two autoionizing states of magnesium by an intense electromagnetic field is investigated experimentally by means of ionization and energy-selected photoelectron spectra probed from the ground state of the atom. The resulting effect of a drastic reduction in the ionization of the system is interpreted as the splitting of the two states achieved through their mixing by the field. A complete theoretical treatment of the problem employing the density matrix formalism is presented, reproducing the effects observed and explaining the phenomenon in terms of the relative populations of the states in the system.
We derive a parametrized formula for the photoionization cross section in the vicinity of an autoionizing state (AIS) coupled with another AIS by a strong laser field. The rotating-wave approximation is used and adiabaticity is assumed. In the probe field spectrum two Fano resonances contribute to the cross section, while a single resonance occurs in the strong-field spectrum. The correlation between the resonance shape and the complex energies of the laser-driven two-level system is described. Calculations are performed for the and AIS pair in He and for the and pair in Mg. The results agree with those obtained using time-dependent approaches. The formula for the cross section describes the spectral features of the ion yield measured in the two-photon ionization of the Mg atom via the AIS coupled with the state. The appearance of laser-induced degenerate states in the cross section shape is studied.
We present experimental results in AC-Stark splitting of an autoionizing state probed by a multiphoton process. In the experiment performed in calcium, the 3d4f 1 P 1 autoionizing state is single-photon coupled with the 4s6s 1 S 0 excited state. The splitting caused by this coupling is probed by three-photon excitation from the ground state. Detuning and laser intensity dependent measurements have been carried out in a collision-free environment. The experimental results can be interpreted and modelled in terms of a few levels system.
We investigate the interaction of ground-state Mg atoms with tuneable laser radiation of ∼5 ns duration and moderate intensity (≤10 12 W cm −2 ), capable of exciting the 3p 2 1 S 0 autoionizing state by four photons. For the corresponding photon energy range, this level is strongly one-photon coupled both with bound (third photon) and, primarily, a multitude of other autoionizing states (fifth photon). The coupling is strong enough to induce the absorption of up to six photons before the atom is ionized, creating thus population into the first excited 3p j Mg + levels which subsequently decay radiatively to the 3s 1/2 ionic ground state. The earlier studies devoted to this excitation scheme were thorough but partial. Particularly, the issues concerning the five-photon excited levels were not addressed. In this work, the examined wavelength range is greatly extended to include these states. Moreover, the interaction is characterized in more detail by employing an array of experimental techniques, namely Mg + ion and photoelectron spectroscopy (including photoelectron angular distributions (PADs) from four- and five-photon ionization) as well as fluorescence spectroscopy where the 3p j →3s 1/2 decay is monitored. The experimental data show that most of these five-photon excited levels undergo blue ac Stark shifts which are occasionally nonlinear with respect to the laser intensity and comparable to or even larger in magnitude than the large redshift of the 3p 2 1 S 0 state itself. Finally, for the latter state, the wavelength dependence of four-photon PAD measurements is suggestive of a situation reminiscent of an ac Stark splitting picture.
Coherent control provides a quantum interference based method for controlling atomic and molecular dynamics. We report two experimental observations of different ways to achieve such a control in atomic photoionization continuum. One is the photoionization of sodium atoms, initially prepared in the 3P1/2 excited state, by a non resonant three-photon interaction with 1064-nm laser light and by a one-photon interaction with the third-harmonic field, at 355 nm. Interference between the two transition paths allows the control of the total ionization rate by varying the relative phase of the laser fields. The second experiment is the observation of the modification of the ionization continua of xenon through laser induced continuum structure (LICS). The multiphoton radiative decay of the xenon ground state into the two electronic continua, that correspond to the two fine structure levels of the ground state of the xenon ion, is varied by electromagnetically embedding a bound state of the atom into the two continua. Both experiments are performed on an atomic beam apparatus which uses a time-of-flight spectrometer for energy analyzing the emitted photoelectrons.