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Journal of Physics B Atomic Molecular and Optical Physics

Resonant two-photon ionization of atoms via two coupled Rydberg series

Niels J. Kylstra, Martin Dörr, C. J. Joachain, Philip George Burke

Published Nov 28, 1995• 18 citations
Publisher

Abstract

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.

DOI
10.1088/0953-4075/28/22/002

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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.
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.
The process of resonant multiphoton ionization of a hydrogen atom in the ground 1 s state is studied by direct numerical integration of the nonstationary Schrödinger equation for a quantum system in an electromagnetic field. The dependence of photoionization probability on the radiation intensity is found to be nonmonotonic. It is established that the minima of ionization correspond to multiphoton resonances between the ground state and one of the excited (Rydberg) atomic states perturbed by the laser field. It is shown that ionization is suppressed due to rearrangement of Rydberg states in a strong electromagnetic field and is accompanied by efficient Raman Λ transitions, which connect a set of closely lying Rydberg states via the continuum.
Within a fully analytically solvable model, we discuss the mechanisms of strong-field suppression of ionization from the initial s state via a family of p Rydberg states to s and d continua. Both Raman coupling via a continuum between different p Rydberg states and Raman migration of population via d continuum from p to higher angular momentum f Rydberg states are considered. The results are compared with those obtained neglecting Raman couplings via the continuum between Rydberg states of the same and different angular momenta. A profound effect of Raman couplings on ionization is demonstrated.
By means of a simple theoretical model and experimental results, we analyse the two-photon ionization of cold rubidium atoms. We consider a two-step process in which ground state atoms are ionized by two blue (421 nm) photons, chosen to be quasi-resonant with the 5S → 6P transition. We show that for a good description of the process we have to take into account not only the three states coupled by the laser radiation, but also all the atomic states involved in the spontaneous emission cascade from the 6P to the 5S state, since optical pumping from 5S 1/2 ( F = 2) to the 5S 1/2 ( F = 1) states modifies the ionization efficiency when ionizing near resonance. The experimental and theoretical determination of ionization cross sections for excitations near resonance with the 6P 1/2 and the 6P 3/2 intermediate levels is presented.
It has been widely believed that short-pulse multiphoton ionization is dominated by a resonance process: excited states of the atom are shifted by the radiation field into multiphoton resonance with the ground state, are populated, and then rapidly ionized. A recent experiment, shows significant population remaining in excited states at the end of the laser pulse, and this result has been interpreted as indicating that ionization proceeds slowly out of these states. We investigate this issue in the framework of Floquet theory, supplemented by direct numerical solution of the time-dependent Schrodinger equation. In this framework, the standard picture is portrayed as an adiabatic transition between Floquet eigenstates, which occurs as the amplitude of the laser field is ramped through the resonance value (i.e. through an avoided crossing of Floquet quasienergies). Thus it follows that the same type of transition must occur as the field is turned off. This mechanism can yield significant populations of excited states that do not suffer appreciable ionization. We exhibit this effect by numerical studies of a model atom with two bound states and two continua.
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