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Physical Review Letters

Redistribution of Rydberg states by intense picosecond pulses

Lambertus D. Noordam, Henrik Stapelfeldt, D. I. Duncan, Thomas F. Gallagher

Published Mar 9, 1992• 80 citations
Publisher

Abstract

Starting with Ba atoms in one Rydberg state we have observed the population of adjacent Rydberg states when the atom is exposed to an intense 1.5-ps laser pulse. The initial Rydberg state population is redistributed by a Raman-like two-photon process, rather than simply being photoionized. This population trapping, which is associated with stabilization against ionization, is described in terms of Rydberg antiwave packets.

DOI
10.1103/physrevlett.68.1496

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Starting with Ba atoms in one Rydberg state we have observed the population of adjacent Rydberg states when the atom is exposed to an intense 1.5-ps laser pulse. The initial Rydberg state population is redistributed by a Raman-like two-photon process, rather than simply being photoionized. This population trapping, which is associated with stabilization against ionization, is described in terms of Rydberg antiwave packets.
We have observed suppression of ionization in Rydberg atoms irradiated by an intense short-pulse laser field. We find that single-photon ionization of the outer electron in a Ba 6snk Stark state can be severely suppressed relative to high-order (\ensuremath{\ge}3 photon) nonresonant multiphoton ionization of the tightly bound 6s core electron. This population trapping occurs in intense short laser pulses, where the bandwidth of the ionizing laser is greater than the spacings between adjacent Stark states, and may be due to a substantial modification of the initial Stark state via stimulated Raman processes through the continuum. The Ba+∗{\mathrm{Ba}}^{+\mathrm{*}}Ba+∗ ion should be left in a higly excited superposition state, or wave packet.
We have observed trapping of population in Rydberg states of atoms and ions exposed to intense laser radiation. The trapping occurs in nonstationary ``wave-packet'' superposition states, created, via ac Stark-shifted multiphoton resonances during the laser pulse. The formation of these highly excited bound states requires the nonresonant absorption of up to 20 or more photons; some of the ionic Rydberg states lie nearly 32 eV above the ionic ground state. All of the trapped states having binding energies much less than the photon energy but remain stable against ionization even when the multiphoton ionization probability of the atom is saturated.
The evolution of a ``dark'' wave packet in Ba is probed using a bound-state interferometric method. The wave packet is created by photoionizing the 5d7d component of a perturbed Rydberg state having predominantly 6snd character, and thereby redistributing population to neighboring states. Information on which Rydberg-Rydberg Raman transitions dominate the transfer of population to each state is obtained. A closed-form expression for the observed strong-field interferograms is developed for the limit of very short pulses. \textcopyright{} 1996 The American Physical Society.
We analyze the excitation of atoms by intense pulsed laser fields and describe a mechanism leading to effective dynamical stabilization at a photon energy below the unperturbed binding energy. At low and intermediate intensities, the atom is left in a coherent superposition of the initial state and a set of Rydberg states which is stable against ionization; this effect subsists for pulse durations presently accessible to experiment. At higher intensities, population is transferred through degenerate Raman coupling to Rydberg states of higher angular momentum.
When exposed to intense light of \ensuremath{\sim}580 nm, the ground state of K shifts up in energy, passing through two-photon resonances with Rydberg states and finally crossing the two-photon ionization limit. Using laser pulses of 0.5 to 13 ps duration, we have shown experimentally that ionization occurs for short pulses, but for long pulses the population is diverted into the Rydberg states where some population survives the peak intensity of the pulse, in excellent agreement with a dynamic Floquet model.
We have studied multiphoton ionization of Ba 6snl Rydberg states by intense ps pulses and have shown that the duration of the laser pulse compared to the orbit time of the Rydberg electron determines the laser-atom interaction. For high-n states with a long orbit time, the loosely bound Rydberg electron is not affected by the intense laser pulse. Instead the inner electron is ejected by absorption of five photons, leaving the Ba+{\mathrm{Ba}}^{+}Ba+ ion in a Rydberg state. For low-n states the outer electron is ejected and the residual Ba+{\mathrm{Ba}}^{+}Ba+ ion can subsequently be multiphoton ionized to Ba++{\mathrm{Ba}}^{++}Ba++.