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Physical Review A

Short-pulse photoionization of perturbed Rydberg states: Laser-induced autoionization

Rutger B. Vrijen, J. H. Hoogenraad, Lambertus D. Noordam

Published Sep 1, 1995• 7 citations
Publisher

Abstract

Laser-induced autoionization, a form of forced autoionization, is discussed. Highly excited atomic Rydberg states generally have a small cross section for photoionization due to their small overlap with the nucleus. The cross section for photoionization can be strongly enhanced if the Rydberg series is perturbed by an atomic state with a relatively large cross section for photoionization. The photoionization dynamics of such a perturbed Rydberg system shows strong similarities to that of an autoionizing Rydberg series. For intense laser pulses, which strongly couple the perturber to the continuum, the photoionization rate is limited by the coupling between the Rydberg states and the perturber or, in other words, the autoionization rate. The model describing this ionization dynamics is applied to the barium 6snd${(}^{1,3}$${\mathit{D}}_{2}$) state which is perturbed by the 5d7d${(}^{1}$${\mathit{D}}_{2}$) state. The calculations show good agreement with experimental results of photoionization of barium Rydberg states with subpicosecond laser pulses of light of 620 nm in wavelength.

DOI
10.1103/physreva.52.2279

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Laser-induced autoionization, a form of forced autoionization, is discussed. Highly excited atomic Rydberg states generally have a small cross section for photoionization due to their small overlap with the nucleus. The cross section for photoionization can be strongly enhanced if the Rydberg series is perturbed by an atomic state with a relatively large cross section for photoionization. The photoionization dynamics of such a perturbed Rydberg system shows strong similarities to that of an autoionizing Rydberg series. For intense laser pulses, which strongly couple the perturber to the continuum, the photoionization rate is limited by the coupling between the Rydberg states and the perturber or, in other words, the autoionization rate. The model describing this ionization dynamics is applied to the barium 6snd{(}^{1,3}$${\mathit{D}}_{2}) state which is perturbed by the 5d7d{(}^{1}$${\mathit{D}}_{2}) state. The calculations show good agreement with experimental results of photoionization of barium Rydberg states with subpicosecond laser pulses of light of 620 nm in wavelength.
The effect of a laser field on the cross section of photoionization of an atom by probe radiation in the region of closely lying autoionizing resonances is studied theoretically. The cross sections in the region of the overlapping autoionizing Rydberg states 5p 5(2 P 1/2)6d′ J = 1 and 5p 5(2 P 1/2)8s′ J = 1 resonantly coupled with the discrete state 5p 5(2 P 3/2)7p[1/2]1 in the xenon atom are calculated. The behavior of the shape and position of resonances in relation to the frequency and intensity of laser radiation is studied.
We have observed that the amount of photoionization from an atomic Rydberg state with a pulsed laser depends critically on the length of the pulse, whereas lowest-order perturbation theory implies that the yield depends only on the fluence (the integrated intensity) of the pulse. We have measured the yield for one-photon ionization with short (0.5–2.7-ps) high-intensity laser pulses from the 27d Rydberg state in barium. With equal fluence, the yield decreases for pulses shorter than the Kepler orbit time of the outer electron (2.2 ps) because not all of its wave function comes near the core during the length of the pulse. The observations and this classical picture are confirmed by quantum-mechanical calculations.
Atoms in doubly excited states above the first ionization limit can decay via autoionization in which an electron is emitted leaving an ion, or by photoemission which leaves the atom in a singly excited state. In this paper, it is demonstrated that interaction between the atoms and a laser pulse that is short compared to the autoionization lifetime can lead to large enhancement of the photoemission process by stimulating the atoms to emit a photon. Since the resultant singly excited atoms do not autoionize, this process can be viewed as an enhancement of the stabilization of the doubly excited atoms against autoionization. A simple theoretical model is outlined that shows good agreement with the experimental results.
We have investigated multiphoton ionization of Ba 6snl6snl6snl Rydberg states by intense 200-fs laser pulses. Specifically, we have excited Ba atoms to the 6sns6sns6sns and 6snd6snd6snd 15\ensuremath{\infty} states using two nanosecond lasers. The atoms were then irradiated with the fs pulses produced by a mode-locked, regeneratively amplified Ti:sapphire laser that is stepwise-tunable between 790 and 850 nm. We have used both the fundamental light and the second harmonic (395--425 nm) to investigate the ionization dynamics in these two wavelength regions. In contrast to previous experiments, in which laser pulses 5 ps or longer were used, our results indicate that excitation of Ba+{\mathrm{Ba}}^{+}Ba+ Rydberg states and Ba2+{\mathrm{Ba}}^{2+}Ba2+ photoions is relatively insensitive to the femtosecond laser wavelength. In addition, we find that, as the Kepler orbital period of the Ba Rydberg electron becomes comparable to this very small laser pulse width, the inner electron ionization process no longer appears to be instantaneous to the outer electron, and the outer electron is not projected onto Ba+{\mathrm{Ba}}^{+}Ba+ Rydberg states.
We describe a detailed account of an experiment demonstrating light-induced stabilization against photoionization. The choice of initial state and atom is discussed in relation to the laser wavelength and laser pulse duration. In combination with a 100-fs, 620-nm probe pulse, the optimum choice is the circular 5g state in neon. A picosecond pump laser was used to prepare this Rydberg state. Initially, the population in this state was probed with a nanosecond laser pulse. Subsequently, the nanosecond probe pulse was replaced by an intense, (sub)picosecond pulse and the photoionization signal was studied. When the probe intensity is several times 1013{10}^{13}1013 W/cm2{\mathrm{cm}}^{2}cm2 a decrease in yield with respect to a less intense pulse with the same fluence is observed, which indicates stabilization. The results are in accordance with recent theoretical predictions.