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Journal of Physics B Atomic Molecular and Optical Physics

Singly, doubly and triply resonant multiphoton processes involving autoionizing states in magnesium

Niels J. Kylstra, H. W. van der Hart, Philip George Burke, C. J. Joachain

Published Jul 28, 1998• 27 citations
Publisher

Abstract

Using the R -matrix Floquet theory we have carried out non-perturbative, ab initio one- and two-colour calculations of the multiphoton ionization of magnesium with the laser frequencies chosen such that the initial state of the atom is resonantly coupled with autoionizing resonances of the atom. Good agreement is obtained with previous calculations in the low-intensity regimes. The single-photon ionization from the excited state of magnesium has been studied in the vicinity of the autoionizing resonance at non-perturbative laser intensities. Laser-induced degenerate states (LIDS) are observed for modest laser intensities. By adding a second laser which resonantly couples the and autoionizing levels, we show that, due to the small width of the state, LIDS occur between this state and the state at intensities of the first laser below . We next investigate the case in which the first laser induces a resonant two-photon coupling between the ground state and the autoionizing state, while the second laser again resonantly couples the respective and autoionizing states. At weak intensities, our calculations compare favourably with recent experimental data and calculations. We show that when the intensity of the first laser is increased, the effect of an additional autoionizing state, the state, becomes significant. This state is coupled to the autoionizing level by one photon, inducing a triply resonant processes. We show that LIDS occur among the three autoionizing levels and we discuss their effect on the decay rate of the ground state. We consider dressed two- and three-level atoms which can be used to model the results of our calculations.

DOI
10.1088/0953-4075/31/14/009

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Using the R -matrix Floquet theory we have carried out non-perturbative, ab initio one- and two-colour calculations of the multiphoton ionization of magnesium with the laser frequencies chosen such that the initial state of the atom is resonantly coupled with autoionizing resonances of the atom. Good agreement is obtained with previous calculations in the low-intensity regimes. The single-photon ionization from the excited state of magnesium has been studied in the vicinity of the autoionizing resonance at non-perturbative laser intensities. Laser-induced degenerate states (LIDS) are observed for modest laser intensities. By adding a second laser which resonantly couples the and autoionizing levels, we show that, due to the small width of the state, LIDS occur between this state and the state at intensities of the first laser below . We next investigate the case in which the first laser induces a resonant two-photon coupling between the ground state and the autoionizing state, while the second laser again resonantly couples the respective and autoionizing states. At weak intensities, our calculations compare favourably with recent experimental data and calculations. We show that when the intensity of the first laser is increased, the effect of an additional autoionizing state, the state, becomes significant. This state is coupled to the autoionizing level by one photon, inducing a triply resonant processes. We show that LIDS occur among the three autoionizing levels and we discuss their effect on the decay rate of the ground state. We consider dressed two- and three-level atoms which can be used to model the results of our calculations.
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.
We present non-perturbative ab initio calculations of resonant two-photon ionization in which the ground state of a complex atom is resonantly coupled by a laser field to two Rydberg states, each of which belongs to a different Rydberg series. As an example, we have studied the resonant two-photon ionization of neon via the 5s and 4d Rydberg states using the R-matrix-Floquet theory. We find that for weak fields, where the Rydberg states are not overlapping, interference effects are already present which lead to a suppression of ionization for a particular laser frequency. For strong fields, the field induced coupling between the two Rydberg states can strongly modify the weak-field behaviour. We give a qualitative explanation of these phenomena by considering the dressed states of a simple three-level model atom coupled to two continua. Finally we show, by varying the intensity, how the Floquet eigenstates corresponding to the ground state and the two Rydberg states of neon are adiabatically connected to the field-free states. © 1995 IOP Publishing Ltd.
We theoretically study intensity-saturation effects in resonant harmonic generation and multiphoton ionization. A first laser excites a two-photon resonance which is coupled by a second laser to an autoionizing state. Starting from an effective Hamiltonian for the three resonant atomic states, we derive a set of equations for the density matrix of the gaseous medium and the electromagnetic field within a semiclassical framework. We present and discuss analytical and numerical solutions of these equations which show a variety of line profiles depending critically on the intensities of the incident laser pulses.
In the present study we have investigated three-photon ionization in Ca in which autoionizing states are engaged. The two-photon resonant process (from the Ca ground state 4s 2 1 S 0 ) occurred through or at least in the vicinity of one of the following states: 4s4d 1 D 2 , 4p 2 3 P 2 , 4s6s 1 S 0 , 4p 2 1 D 2 and 4p 2 1 S 0 , with the third photon either reaching the continuum directly or one of the autoionizing states. The three-photon resonant transitions to 3d m p, m f: 1 P 1 , 3 P 1 and 3 D 1 autoionizing states for m up to 21 have been observed. Some of the autoionizing resonances which we have found had not been observed before in a high-resolution one-photon absorption experiment (for J = 1) and in multiphoton experiments (for J = 3). We have compared the ionization signal as a function of the laser detuning and the laser intensity with theoretical curves obtained within a simple model (three-level atom + one-mode laser field). This gives information about the order of magnitude of the three-photon ionization probability through autoionizing states.
We study double-resonance processes in Magnesium.One laser is used to "pump" the 3p2 resonance through two-photon absorption from the 3s^ fundamental state of Mg.A second laser couples the 3p^ l se resonance to the 3p3d lp° narrow autoionizing state.In the experiment the ionization rate is measured in two different situations; with a fixed frequency for the pumping (coupling) laser and varying the frequency of the coupling (pumping) laser.In agreement with the experimental findings, a theoretical study shows that, for particular frequencies of the laser fields, a situation of coherent trapping occurs with a partial stabilization of 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.