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Physical Review A

Configuration interaction and Raman redistribution in perturbed Ba Rydberg states

Michael L. Bajema, Robert van Leeuwen, Elena Murgu, Thomas F. Gallagher

Published Jan 14, 2000• 2 citations
Publisher

Abstract

We have experimentally observed the time dependence of the population oscillation between a doubly excited state and singly excited Rydberg states subsequent to excitation by a short laser pulse. Specifically, we have examined the case in which the configuration interaction between a doubly excited state and a singly excited Rydberg series is weak. The data are quantitatively reproduced using a quantum defect theory calculation, and we contrast simple classical pictures of the population oscillation for weak and strong configuration interaction. We also observe significant, and unexpected, Raman redistribution by the final laser pulse, and we are able to demonstrate that it occurs primarily by Raman transitions via a lower state, not via the continuum.

DOI
10.1103/physreva.61.023414

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We have experimentally observed the time dependence of the population oscillation between a doubly excited state and singly excited Rydberg states subsequent to excitation by a short laser pulse. Specifically, we have examined the case in which the configuration interaction between a doubly excited state and a singly excited Rydberg series is weak. The data are quantitatively reproduced using a quantum defect theory calculation, and we contrast simple classical pictures of the population oscillation for weak and strong configuration interaction. We also observe significant, and unexpected, Raman redistribution by the final laser pulse, and we are able to demonstrate that it occurs primarily by Raman transitions via a lower state, not via the continuum.
Using the optical Ramsey method we have observed the configuration interaction in Ba drive atoms back and forth between the doubly excited 5d7d state and the degenerate 6snd Rydberg states. Our observations can be understood qualitatively as autoionization of the initially excited 5d7d state into the Rydberg states, followed by capture of the Rydberg electron by the ion a Kepler time later. After a time delay, the whole process repeats. A quantum defect theory description provides a quantitative picture and clarifies the connection to resonance scattering.
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.
Following the experiment of Jones et al. [Phys. Rev. Lett. 71, 2575 (1993)], we present a theory of coherent redistribution of population in a model Rydberg atom exposed to a sequence of two identical laser pulses separated in time and shorter in duration than the Rydberg-electron Kepler period. For different initial-population conditions, we solve the problem of redistribution in a fully analytical and rigorously nonperturbative way, thus obtaining discrete-state population amplitudes, dependent on laser intensity, and a time delay between the pulses. Using this solution, we study the population in a given state versus pulse delay (Ramsey fringes), as well as the corresponding Fourier spectrum, for both low and high laser intensities. From the number of frequency components and their positions in the Fourier spectrum, we deduce the redistribution of the initial-state population over a number of states by the first pulse. Within our model calculations we achieve qualitative agreement with the experimental observation of Jones et al. that an increase in laser intensity results in a general increase in the number of frequency components in the Fourier spectrum. Our theoretical results are also consistent with the experimental finding of Noordam et al. [Phys. Rev. Lett. 68, 1496 (1992)] that Raman transitions via the continuum between different Rydberg states are essential for population redistribution. We suggest new experiments to measure the effect of the initial-state depletion on the Fourier spectrum. As follows from our model calculations, some frequency components (both low and optical) present in the low-intensity Fourier spectrum should vanish in the high-intensity spectrum due to complete depletion of the initial state by the first pulse.
Our recent approximate analytical results on the evolution of the initial state and the excitation from this state of a band of high Rydberg states by an optical pulse [Phys. Rev. A 55, 2144 (1997)] are compared with more exact numerical results. The difference between the two approaches is that the approximations of representative atom-field couplings and equidistant spacing of high Rydberg states, applied in the analytical model, are removed in the numerical model. We find that the approximate analytical model is not able to reproduce all the results of the more exact numerical model, if the laser pulse is very short (i.e., much shorter that the Kepler period of the resonantly excited high Rydberg state) or very intense (i.e., when the Rabi period for the resonant transition is substantially shorter than the above Kepler period). This mainly concerns the redistribution of the population over different Rydberg states. The analytical model predicts a symmetric distribution centered around the resonantly excited Rydberg state, irrespective of the pulse duration and intensity, while the numerical model allows an asymmetric distribution with its maximum shifted towards lower Rydberg states. Despite the above-stated difference, the analytical model is able to give preliminary results for the total population of all the excited Rydberg states and the evolution of the initial state, imitating at least qualitatively the results of the numerical model in certain time and intensity scales.