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Physical Review Letters

Rydberg-Rydberg Collisions: Resonant Enhancement of State Mixing and Penning Ionization

Aaron Reinhard, Tara Cubel Liebisch, Kelly Cooper Younge, P. R. Berman, Georg A. Raithel

Published Mar 28, 2008• 61 citations
Publisher

Abstract

In rubidium Rydberg states, the collision nD_(5/2)+nD_(5/2)-->(n-2)F_(7/2)+(n+2)P_(3/2) is nearly resonant in the vicinity of n=43. As a result, over a short range of n centered around n approximately 43 the Rydberg-Rydberg interaction potential is quite large and turns from repulsive to attractive [Phys. Rev. A 75, 032712 (2007)10.1103/PhysRevA.75.032712]. We use state-selective field ionization to investigate the effect of this resonance on instantaneous excitation of mixed two-particle states, state-mixing collisions, and Penning ionization. We find that these processes depend on the magnitude and sign of the two-particle interaction potential, and thus on n near the resonance. The large magnitude of the observed state mixing provides evidence for many-body effects.

DOI
10.1103/physrevlett.100.123007

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In rubidium Rydberg states, the collision nD_(5/2)+nD_(5/2)-->(n-2)F_(7/2)+(n+2)P_(3/2) is nearly resonant in the vicinity of n=43. As a result, over a short range of n centered around n approximately 43 the Rydberg-Rydberg interaction potential is quite large and turns from repulsive to attractive [Phys. Rev. A 75, 032712 (2007)10.1103/PhysRevA.75.032712]. We use state-selective field ionization to investigate the effect of this resonance on instantaneous excitation of mixed two-particle states, state-mixing collisions, and Penning ionization. We find that these processes depend on the magnitude and sign of the two-particle interaction potential, and thus on n near the resonance. The large magnitude of the observed state mixing provides evidence for many-body effects.
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.
Using state-selective field ionization, the state distributions of Rydberg atoms in cold Rydberg gases are measured for various initially excited Rydberg levels, populations, and evolution times. We provide direct experimental evidence for lll-changing collisions that we previously observed indirectly [S. K. Dutta, D. Feldbaum, A. Walz-Flannigan, J. R. Guest, and G. Raithel, Phys. Rev. Lett. 86, 3993 (2001)]. We also observe nnn-mixing and find that its effects are largely in agreement with recent theoretical work on nnn-changing collisions between electrons and Rydberg atoms, thus enabling an estimation of the electron temperature. Unexpectedly large populations of atoms are found in states with principal quantum numbers much lower than that of the initially excited atoms. We explain this observation by collisions between high-lll Rydberg atoms, which are highly polar and can collide due to static electric-dipole forces between them.
Systems of cold, interacting Rydberg atoms are of interest because they exhibit a wide range of collective quantum phenomena. This thesis describes experimental and theoretical work related to these systems with an emphasis on two phenomena: Rydberg excitation blockades and quantum-state-changing collisions. I begin by presenting a detailed calculation of the interaction energies of two Rydberg atoms for a variety of orientations, quantum states, and applied electric fields. The calculated energies are used to interpret the experimental results that follow. I then describe measurements showing that the widths of the distributions of Rydberg excitation number are related to the effectiveness of a Rydberg excitation blockade. These distributions are investigated as a function of principal quantum number, n, and applied electric field. In the presence of a Forster resonant field, sub-Poissonian distributions are measured. I next present a spectroscopic measurement of the energy level shift of a system of atoms which collectively shares two Rydberg excitations. The qualitative nature of the shift depends sensitively on the type of interactions between the atoms (van der Waals or dipole-dipole) and may be changed by changing the quantum state or applied electric field. This measurement provides the first spectroscopic proof that Rydberg excitation blockades are operative. Finally, I describe measurements of the probability for quantum state-changing and Penning-ionizing collisions to provide evidence for intrinsic, electric field-free-interaction resonances and complex many-body interactions in systems of cold Rydberg atoms.
In a recent work [Phys. Rev. Lett. 98, 023004 (2007)], we investigated the influence of the attractive van der Waals interaction on the pair distribution and Penning ionization dynamics of ultracold Rydberg gases. Here we extend this description to atoms initially prepared in Rydberg states exhibiting repulsive interaction. We present calculations based on a Monte Carlo algorithm to simulate the dynamics of many atoms under the influence of both repulsive and attractive long-range interatomic forces. Redistribution to nearby states induced by blackbody radiation is taken into account, changing the effective interaction potentials. The model agrees with experimental observations, where the ionization rate is found to increase when the excitation laser is blue detuned from the atomic resonance.
We have observed the sharply resonant enhancement of the cross section of the collision process $ns+ns\ensuremath{\rightarrow}np+(n\ensuremath{-}1)p$ between two Nans\mathrm{Na}nsNans (16< n< 2716<~n<~2716< n< 27) atoms which occurs when the levels are shifted by an electric field so that the nsnsns level lies midway between the two ppp states. The widths of the collisional resonances scale as ${n}^{\ensuremath{-}2}$ and the magnitudes of the cross sections as n4{n}^{4}n4, with values of 0.5 GHz and 8\ifmmode\times\else\texttimes\fi{}108{10}^{8}108 A˚2{\mathrm{\AA{}}}^{2}A˚2 for the 20s20s20s state. These results are in good agreement with calculations based on the long-range dipole-dipole interaction between the two atoms.