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Physical Review Letters

Formation of Rydberg Atoms in an Expanding Ultracold Neutral Plasma

T. C. Killian, M. J. Lim, S. A. Kulin, Rainer Dumke, Scott Bergeson, S. L. Rolston

Published Apr 23, 2001• 257 citations
Publisher

Abstract

We study the formation of Rydberg atoms in expanding plasmas at temperatures of 1-1000 K and densities from 10(5)-10(10) cm(-3). Up to 20% of the initially free charges recombine in about 100 micros, and the binding energy of the Rydberg atoms approximately equals the increase in the kinetic energy of the remaining free electrons. Three-body recombination is expected to dominate in this regime, yet most of our results are inconsistent with this mechanism.

DOI
10.1103/physrevlett.86.3759

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We study the formation of Rydberg atoms in expanding plasmas at temperatures of 1-1000 K and densities from 10(5)-10(10) cm(-3). Up to 20% of the initially free charges recombine in about 100 micros, and the binding energy of the Rydberg atoms approximately equals the increase in the kinetic energy of the remaining free electrons. Three-body recombination is expected to dominate in this regime, yet most of our results are inconsistent with this mechanism.
By photoionizing a sample of laser-cooled xenon atoms, we create ultracold neutral plasmas with initial temperatures of 1–1000 K and densities as high as 1010 cm−3. The plasma is formed by the trapping of electrons by the residual positive charge that is left after some electrons initially leave the sample. We excite plasma oscillations with applied radio frequency fields and use this to monitor the expansion of the unconfined plasma. We have observed significant recombination of the plasma into Rydberg atoms (up to 20%). At these low temperatures, the only traditional form of recombination that could be significant is three-body recombination (TBR), but we see a number of trends in direct contradiction to what one would expect from classical TBR theory.
Summary form only given. We have observed recombination into a large range of Rydberg levels in an ultracold plasma. The plasma is created by two-photon ionization of laser-trapped and -cooled metastable xenon atoms. By changing the intensity and detuning of the ionizing laser pulse, the initial temperature and density of the plasma can be varied. This allows us to access plasma coupling parameters (???) between 0.1 and 5. In this range of values, we previously reported unexplained heating of the expanding cloud, between 10 and 100 ???s after creation of the plasma. The recently observed recombination appears to provide much of the extra energy responsible for this behavior. The recombined atoms, up to 20% of the created plasma, populate energy levels down to n=40. They survive for /spl sim/1 ms indicating that high angular momentum states are present. However, standard scaling laws for three-body recombination do not agree with the observed dynamics. Furthermore, Rydberg atom formation is incomplete at the time when the plasma expansion velocity has reached its maximum value. Various effects are under consideration as possible remedies to these inconsistencies.
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.
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.
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.
In plasmas at very low temperatures, the formation of neutral atoms is dominated by collisional three-body recombination, owing to the strong $\ensuremath{\sim}{T}^{\ensuremath{-}9/2}$ scaling of the corresponding recombination rate with the electron temperature TTT. While this law is well established at high temperatures, the unphysical divergence as $T\ensuremath{\rightarrow}0$ clearly suggests a breakdown in the low-temperature regime. Here, we present a combined molecular dynamics Monte Carlo study of electron-ion recombination over a wide range of temperatures and densities. Our results reproduce the known behavior of the recombination rate at high temperatures, but reveal significant deviations with decreasing temperature. We discuss the fate of the kinetic bottleneck and resolve the divergence problem as the plasma enters the ultracold, strongly coupled domain.