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The Journal of Chemical Physics

n-changing population of Rydberg states by low-energy electron–Rydberg collisions

Yufan Li, Feng Fang, Wenchang Zhou, Dingming Liu, Zhangru He, Dongmei Zhao, Bennaceur Najjari, Jie Yang

Published Oct 8, 2024• 0 citations
Publisher

Abstract

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.

DOI
10.1063/5.0231333

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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.
Rydberg atom formation is a source of heating in plasmas. The rate of three-body recombination in an ultracold neutral plasma was measured and electron temperature was derived from it using standard equilibrium recombination rates. With large-scale Monte Carlo and particle-in-cell simulations, we have calculated ab initio the rate of excitation, de-excitation, ionization (and recombination) in electron-Rydberg atom collision and investigated the short-time dynamics of three-body recombination in an ultracold neutral plasma. Comparison with observed rates is quite good. Particular attention is paid to the low-frequency microfield effect on Rydberg state cut-off in the plasma.
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.
Rydberg atom formation is a source of heating in plasmas. The rate of three-body recombination in an ultracold neutral plasma was measured and temperature for the plasma was extracted. With large-scale Monte Carlo and particle-in-cell simulations, we have ab initio calculated the rate of excitation, de-excitation, ionization (and recombination) in electron-Rydberg atom collision and investigated the short-time dynamics of three-body recombination in an ultracold neutral plasma. Comparison with observed rates is quite good. Particular attention is paid to the low-frequency microfield effect on Rydberg state cut-off in the plasma.
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.
The details of recent calculations of the expansion of ultra-cold, neutral plasmas are given. The calculations are performed at several levels. The simplest level assumes an ansatz for the form of the electron and ion density; the result is a simple, ordinary differential equation which can be easily solved. The medium level of sophistication assumes the electrons are in thermal equilibrium but does not assume a particular form for the ion density; the result is a partial differential equation which is solved numerically. For the highest level of sophistication, a Monte Carlo technique is used to solve for the electron phase space distribution and solve for the ion motion in the resulting mean field. All levels of simulation include three body recombination and electron-Rydberg scattering. This paper contains the results of our simulations and compares them to measurements made on ultra-cold plasmas. Three body recombination is found to be important at very low temperatures since it is a heating mechanism for the electron gas. The collisions between cold electrons and Rydberg atoms are another important source of electron heating and de-excitation of atoms formed in the plasma. The evolution of the distribution of atoms in the plasma is simulated and several counter-intuitive effects that have been observed can be explained. Our simulations show that the plasma coupling constant does not become larger than ∼1/5 for the reported experiments. The behavior of plasma processes are investigated, e.g., ion acoustic waves, spike formation, and electron evaporation. The evolution of a cold Rydberg gas into a plasma is also simulated but certain properties of our simulation do not agree with measurements.
Signals of ultracold plasma are observed by two-photon ionization of laser-cooled caesium atoms in a magneto-optical trap. Recombination of ions and electrons into Rydberg atoms during the expansion of ultracold plasma is investigated by using state-selective field ionization spectroscopy. The dependences of recombination on initial electron temperature (1–70 K) and initial ion density (∼10 10 cm −3 ) are investigated. The measured dependence on initial ion density is N 1.547+0.004 at a delay time of 5 μs. The recombination rate rapidly declines as initial electron temperature increases when delay time is increased. The distributions of Rydberg atoms on different values of principal quantum number n, i.e. n = 30–60, at an initial electron temperature of 3.3 K are also investigated. The main experimental results are approximately explained by the three-body recombination theory.