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Journal of Physics B Atomic Molecular and Optical Physics

Time-resolved configuration interaction

Douglass W. Schumacher, D. I. Duncan, R. R. Jones, Thomas F. Gallagher

Published Jun 14, 1996• 24 citations
Publisher

Abstract

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.

DOI
10.1088/0953-4075/29/11/002

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Physical Review A•Jun 1, 1981•52 citations
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.
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.
We report the observation of doubly excited autoionizing Rydberg states of Sr, belonging to the configuration 5p125{p}_{\frac{1}{2}}5p21​​, nl\mathrm{nl}nl. Our procedure involves a three-step optical excitation process which incorporates Stark switching to reach higher lll states not normally accessible because of dipole selection rules. Quantum defects are reported for several 5p125{p}_{\frac{1}{2}}5p21​​, ns\mathrm{ns}ns and 5p125{p}_{\frac{1}{2}}5p21​​, nd\mathrm{nd}nd states. The lifetimes of the 5p125{p}_{\frac{1}{2}}5p21​​, ns\mathrm{ns}ns states are shown to scale as (n∗)3{({n}^{*})}^{3}(n∗)3, and the lifetimes of the 5p125{p}_{\frac{1}{2}}5p21​​, 16l16l16l states are shown to increase dramatically with increasing lll.
Rydberg atoms are increasingly being used as a means of introducing long-range, tunable interactions into atomic systems through their strong dipole-dipole interactions. When creating such interactions, however, there are a variety of potential effects that can occur, such as state (n and/or L) changing or Penning ionization, which can complicate the dynamics of the system. In the following work, such interactions are investigated for Rydberg-Rydberg collisions using very high-n, n ~300, strontium Rydberg atoms in an atomic beam configuration. By exploiting Rydberg blockade and the inherent distribution of atomic velocities present in an atomic beam, it is possible to create a 1D array of moving Rydberg atoms which will naturally overtake each other over time. Measurements of both Penning ionization and state changing for such collisions are made and compared with classical trajectory Monte-Carlo (CTMC) simulations, with both indicating large collisional cross sections on the order of 1 x 10-6 cm2 for Penning ionization and nearly 8 x 10-5 cm2 for state changing interactions. In a second series of experiments, previous work involving doubly-excited Rydberg states is expanded upon by investigating autoionization with high-n, L > 3, Rydberg states. Past research involving autoionization has shown that the effect is strongly L-dependent, with high-L states having significantly smaller autoionizing rates. To create well-defined, L > 3 states, the use of microwave fields to drive various high-n, n ~ 150, n1F3 → (n+1)1G4, (n+2)1H5 transitions is investigated, with spectroscopic measurements of these transitions providing quantum defect values for n1G4 and n1H5 states. These measurements provide a basis for future studies into the L-dependence of high-n, n ~ 300, autoionizing Rydberg atoms, with the eventual goal of creating a long-lived, doubly-excited “planetary” Rydberg state.
To probe the configuration mixing between the Ba 6snd1D26snd^{1}D_{2}6snd1D2​ and 3D2^{3}D_{2}3D2​ Rydberg series and the 5d7d1D25d7d^{1}D_{2}5d7d1D2​ perturber we have observed the radio-frequency transitions between the 5d7d1D25d7d^{1}D_{2}5d7d1D2​ state and the 6s28s1S06s28s^{1}S_{0}6s28s1S0​, 6s24f3F26s24f^{3}F_{2}6s24f3F2​, and 6s24f1F36s24f^{1}F_{3}6s24f1F3​ states using a delayed-field-ionization approach. The transitions are observed in the presence of small (\ensuremath{\sim}1 V/cm) electric fields, and from the Stark shifts of the transitions we are able to estimate the 1D^{1}D1D and 3D^{3}D3D Rydberg fractions of the 5d7d5d7d5d7d state. Our measured zero-field term separations tie together previous optical measurements of the various Rydberg series involved. In addition, we have measured the lifetimes of the 6snd6snd6snd states in the vicinity of the 5d7d5d7d5d7d perturber to estimate the fraction of 5d7d5d7d5d7d character in each of the Rydberg states. The values we find for the configuration mixing are in reasonable agreement with those determined by a multichannel-quantum-defect-theory analysis of the optical spectrum of the even-parity J=2J=2J=2 states of Ba.