Synopsis State-changing in thermal-energy collisions between strontium atoms in high-n, n∼300, n1F3 Rydberg states is studied in an atomic beam and analyzed using classical trajectory Monte Carlo simulations. The L-changing cross section is large, ∼10-4 cm2, much greater than the corresponding “hard-sphere” cross section.
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.
State changing in thermal-energy collisions between strontium atoms in very-high-n, $n\ensuremath{\approx}300$, n1F3 Rydberg states is studied. In collisions between Rydberg atoms, the dipole-dipole interaction generates an effective electric field at each atom, which triggers Stark precession and the evolution of their angular momenta, L. Such L-changing collisions are examined using both quantum and classical theory. The theoretical predictions are experimentally verified by monitoring the damping of quantum beats induced by the sudden application of a DC ``pump'' field. The present work shows that, due to the long-range nature of the interactions, the cross sections, $\ensuremath{\sigma}$, for L changing are considerably larger than the geometric collision cross section. For thermal collisions the cross section $\ensuremath{\sigma}$ for n1F3 Rydberg states with $n\ensuremath{\simeq}300$ is $\ensuremath{\approx}8\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}5}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{2}$. Scaling rules derived in this paper predict that for cold collisions $\ensuremath{\sigma}$ may increase by a further factor of 4.
The destruction of high-$n, n\ensuremath{\sim}300$, strontium atoms contained in a hot atomic beam through Rydberg-Rydberg collisions is examined. The Rydberg atoms are initially created, under blockade conditions, in a localized volume and their subsequent motions lead to creation of a string of Rydberg atoms. The Rydberg atoms, however, are formed with a thermal distribution of velocities resulting in Rydberg-Rydberg collisions which lead to their destruction. The experimental data are interpreted using classical trajectory Monte Carlo techniques that simulate the excitation of the Rydberg atoms together with their subsequent motions. Using calculated collisional ionization cross sections and blockade radii, the model yields results in good agreement with experiment. The results highlight the important role collisional destruction can play when attempting to study (long-range) Rydberg-Rydberg interactions in a hot atomic beam.
Semiclassical calculations of the quasi-elastic l-mixing and inelastic n,l-changing processes in thermal collisions of a Rydberg sodium atom with rare-gas atoms (Ne, Ar, Kr and Xe) as well as and atoms with Ne are presented in a wide range of principal quantum numbers. The main emphasis is put on the study of the effects in the Rydberg-atom - rare-gas-atom collisions associated with both the short- and long-range (polarization) parts of the electron - perturber interaction. It is shown that the polarization interaction between the highly excited electron and the Ne atom provides the major contribution to the cross section of the l-mixing and n, l -changing transitions. We show that the Ramsauer - Townsend effect in slow electron scattering by the heavy rare-gas atoms significantly affects the values of the cross sections, particularly for the inelastic transitions with large energy transfer. A quantitative explanation of these phenomena is given using the recently developed semiclassical normalized perturbation theory for the Rydberg-atom - neutral collisions combined with the modified effective range theory for scattering of slow electrons by the rare-gas atoms.
In thermal-energy collisions between sodium atoms in ns or np states (32<n<52) and xenon atoms, depopulation of the Rydberg states is observed to occur predominantly through state-changing reactions of the type $\mathrm{Na}(ns or np)+\mathrm{Xe}\ensuremath{\rightarrow}\mathrm{Na}(n\ensuremath{-}1, l>~2)+\mathrm{Xe}$. For the present range of n, the measured cross sections increase with n and lie between 1500 and 2600 A˚2 for ns states and between 2000 and 4200 A˚2 for np states. Implications of the data are discussed.
State-changing in collisions of Rb(nS) - HF are studied using a crossed atomic beam/modulated CW laser technique and selective field ionization for values of principal quantum number n where 40 (LESSTHEQ) n (LESSTHEQ) 49. Collisions between a rotating polar molecule and a Rydberg atom often result in a near-resonant interchange of the rotational energy of the molecule, and a corresponding change in the electronic energy of the atom. A critical parameter is the energy imbalance of the reaction, defined as the difference between the atom's initial and final electronic energy and the molecule's initial and final rotational energy. The molecule used in this experiment, hydrogen fluoride, has a large rotational constant which permits study of n-changing rate constants for transitions from an initially populated s-state to a single n-manifold of high-L states. Because only one final manifold is populated, the reaction involves a single energy imbalance, and thus proves a useful test of theoretical models. n-Changing rate constants for collisions with energy imbalances ranging from 0.057 cm('-1) to 3.447 cm('-1), and ionization and L-mixing rate constants are compared to those predicted by an impulse approximation model and a semiclassical approach.