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Physical Review A

Rydberg transitions induced by optical core dressing

N. J. van Druten, Harm Geert Muller

Published Oct 1, 1995• 9 citations
Publisher

Abstract

We study theoretically the behavior of two atomic Rydberg series, coupled by a light field that strongly drives the optical transition between the core states to which these series converge. It is shown that this strong-field version of isolated-core excitation leads to a strong modification of the photoionization spectrum and to transitions between adjacent Rydberg states when the Rabi frequency associated with the core transition becomes larger than the Rydberg spacing. The intensities and pulse durations (\ensuremath{\approx} 2 GW/cm2 and 1 ps, respectively, for $n\ensuremath{\approx}20$ Rydberg states) needed for the observation of these effects are within reach of present-day lasers.

DOI
10.1103/physreva.52.3047

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Physical Review Research•May 19, 2022•10 citations
We study theoretically the behavior of two atomic Rydberg series, coupled by a light field that strongly drives the optical transition between the core states to which these series converge. It is shown that this strong-field version of isolated-core excitation leads to a strong modification of the photoionization spectrum and to transitions between adjacent Rydberg states when the Rabi frequency associated with the core transition becomes larger than the Rydberg spacing. The intensities and pulse durations (\ensuremath{\approx} 2 GW/cm2 and 1 ps, respectively, for n\ensuremath≈20n\ensuremath{\approx}20n\ensuremath≈20 Rydberg states) needed for the observation of these effects are within reach of present-day lasers.
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{(}^{1,3}(1,3D2{\mathit{D}}_{2}D2​) state which is perturbed by the 5d7d(1{(}^{1}(1D2{\mathit{D}}_{2}D2​) 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.
Excitation and photoionization of Rydberg wave packets are described. Interference of bound-free transitions from many coherently populated Rydberg levels is shown to affect the dependence of the photoionization probability on the duration of interaction. Strong-field interference effects in such a system are described also. The most important of these is the field-induced interference stabilization of Rydberg atoms in a strong ionizing field. The intensity range in which this effect can exist is determined. The results derived are used for a qualitative model describing supercontinuum emission in the process of multiphoton ionization.
We develop a theory describing laser excitation of a Rydberg series by an intense laser field. Our theory is based on the fact that the radiative coupling is restricted to a region around the atomic nucleus (the reaction zone) which is small in comparison with the extent of the excited Rydberg states. The physical processes inside the reaction zone are characterized by a few parameters which are slowly varying functions of energy across the Rydberg threshold. This finite range of the radiative coupling allows us to apply methods from quantum-defect theory and to treat the laser interaction with the Rydberg series and the adjoining electron continuum as a whole. Within this approach we derive analytical expressions for transition probabilities as a function of time in either a dressed-state representation which is appropriate as long as only a few Rydberg states are excited or a multiple-scattering expansion which is particularly suited for a description of the excitation process close to threshold. The physical picture emerging in this limit is one of a radial electronic wave packet which is generated within the reaction zone and moves in the Coulomb potential of the ionic core. Every time it returns to the inner turning point of its orbit, i.e., to the reaction zone, it is either deexcited back to the initial atomic state or is scattered by the ionic core.
We study the dynamics of an atomic Bose-Einstein condensate in an optical lattice in which the electronic ground state of each atom is weakly coupled to a highly excited Rydberg state by a far off-resonant laser. This dressing induces a switchable effective soft-core interaction between ground-state atoms which, in the lattice, gives rise to on-site as well as long-range interaction terms. Upon switching on the dressing laser the coherence properties of the atomic superfluid undergo a nontrivial collapse and revival dynamics which can be observed in the interference pattern that is created after a release of the atoms from the optical lattice. This interference signal strongly depends on the strength and the duration of the dressing laser pulse and can be used to probe and characterize the effective interaction between Rydberg-dressed atoms.
The AC Stark shift of electronic levels is ubiquitous in the interaction of intense light fields with atoms and molecules. As the light intensity changes on the rising and falling edges of a femtosecond laser pulse, it shifts the Rydberg states in and out of multiphoton resonances with the ground state. The two resonant pathways for transient excitation arising at the leading and the trailing edges of the pulse generate Young's type interference, generally referred to as the St\"uckelberg oscillations. Here we report the observation of the St\"uckelberg oscillations in the intensity of the coherent free-induction decay following resonant multiphoton excitation. Moreover, combining the experimental results with accurate numerical simulations and a simple model, we use the St\"uckelberg oscillations to recover the population dynamics of strongly driven Rydberg states inside the laser pulse by all-optical measurements after the end of the pulse. We demonstrate the potential of this spectroscopy to characterize lifetimes of Rydberg states dressed by laser fields with strengths far exceeding the Coulomb field between the Rydberg electron and the core.