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Physical Review A

Cold-Rydberg-gas dynamics

Alisa I. Walz‐Flannigan, Jeffrey R. Guest, Jongsoo Choi, Georg A. Raithel

Published Jun 7, 2004• 85 citations
Publisher

Abstract

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 $l$-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 $n$-mixing and find that its effects are largely in agreement with recent theoretical work on $n$-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-$l$ Rydberg atoms, which are highly polar and can collide due to static electric-dipole forces between them.

DOI
10.1103/physreva.69.063405

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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.
We have observed the evolution of cold Rydberg gases and ultracold plasmas in an environment that allows for the control of interactions of the blackbody radiation temperature from 4K to 300K. The work in this thesis describes the influence of initial densities, populations, excitation state, evolution time and thermal background temperature on the evolution of cold Rydberg gases as well as directly excited ultracold plasmas. With some initial ionization, cold-Rydberg-atom gases easily develop a positive space charge that traps electrons for times on the order of tens of mus. This acts as a catalyst for electron-Rydberg atom collisions, increasing the collision probabilities by orders of magnitude and profoundly altering the final state of the Rydberg gas. Using state-selective field ionization, we have provided direct proof that these collisions cause changes in l-states, and we have seen the first experimental evidence that they also lead to inelastic n-changing collisions, as predicted by theory. We have also found evidence for Rydberg-Rydberg collisions, enabled by the attractive electric-dipole forces between atoms in high-l states and possibly by van-der-Waal's interactions at very high-n . Thermal interactions are seen to influence the formation of a plasma from a cold Rydberg gas. Plasmas form more easily in the presence of a 300K radiation field than at 4K, due to the contribution of thermal ionization to the plasma formation. The background temperature also appears to affect the electron temperature in both the directly excited plasma and the plasma spontaneously formed from a cold Rydberg gas. In Rydberg atom gases that have undergone partial ionization, electron temperatures were estimated using the dependence of n-changing collisions on the electron temperature.
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.
Cold, dense Rydberg gases produced in a cold-atom trap are investigated using spectroscopic methods and time-resolved electron counting. Optical excitation on the discrete Rydberg resonances reveals long-lasting electron emission from the Rydberg gas ( >20 ms). Our observations are explained by lm-mixing collisions between Rydberg atoms and slow electrons that lead to the population of long-lived high-angular-momentum Rydberg states. These atoms thermally ionize slowly and with large probabilities.
Dense samples of cold Rydberg atoms have previously been observed to spontaneously evolve to a plasma, despite the fact that each atom may be bound by as much as $100\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$. Initially, ionization is caused by blackbody photoionization and Rydberg-Rydberg collisions. After the first electrons leave the interaction region, the net positive charge traps subsequent electrons. As a result, rapid ionization starts to occur after $1\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{s}$ caused by electron-Rydberg collisions. The resulting cold plasma expands slowly and persists for tens of microseconds. While the initial report on this process identified the key issues described above, it failed to resolve one key aspect of the evolution process. Specifically, redistribution of population to Rydberg states other than the one initially populated was not observed, a necessary mechanism to maintain the energy balance in the system. Here we report new and expanded observations showing such redistribution and confirming theoretical predictions concerning the evolution to a plasma. These measurements also indicate that, for high nnn states of purely cold Rydberg samples, the initial ionization process which leads to electron trapping is one involving the interactions between Rydberg atoms.
Inelastic n-changing collisions play an important role in the evolution of Rydberg atoms into ultracold plasmas. However, for the initially intermediate n (n ∼ 40) Rydberg states, these collisions can hardly be observed due to the low electron temperature in ultracold plasmas. In this work, we designed an experimental scheme to facilitate collisions between free electrons at 1.5 eV and intermediate n Rydberg atoms. Using the field ionization technique, we measured the state distributions resulting from the evolution of initially cold rubidium atoms in the 45P3/2 Rydberg state. The experimentally obtained probability of inelastic collisions excitation agrees well with the Monte Carlo simulation results. In addition, our experimental results indicate that the n-changing population induced by hot electrons is significant for lower nP Rydberg states. Our work plays a significant role in calculating the rates of electron-ion three-body recombination in ultracold plasmas.
Cold, dense Rydberg gases produced in a cold-atom trap are investigated using spectroscopic methods and time-resolved electron counting. On the discrete Rydberg resonances we observe large trap losses and long lasting electron emission from the Rydberg gas (>30ms). Our observations are explained by quasi-elastic l-mixing collisions between Rydberg atoms and slow electrons that lead to the population of long-lived high-angular-momentum Rydberg states. These atoms thermally ionize slowly and with large probabilities, leading to the observed effects.