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Physical Chemistry Chemical Physics

Molecular ion–electron recombination in an expanding ultracold neutral plasma of NO+

Hossein Sadeghi, Markus Schulz-Weiling, J. P. Morrison, Julian C. H. Yiu, Nicolas Saquet, Chris Rennick, Edward R. Grant

Published Jan 1, 2011• 20 citations
Publisher

Abstract

Using state-selected double-resonant excitation, we create a Rydberg gas of NO molecules excited to the principal quantum number n = 50 of the f-series converging to the ion rotational level, N(+) = 2. This gas evolves to form an ultracold plasma, which expands under the thermal pressure of its electrons, and dissipates by electron-ion recombination. Under conditions chosen for this experiment, the observed rates of expansion vary with selected plasma density. Electron temperatures derived from these expansion rates vary from T(e) = 12 K for the highest density up to 16 K at four-fold lower density. Over this range, the apparent electron coupling parameter, defined as Γ(e) = e(2)/4πε(0)ak(B)T(e), falls from nearly three to about one. The decay of charged-particle density fits with a kinetic model that includes parallel paths of direct two-body and stepwise three-body dissociative recombination. The overall recombinative decay follows a second-order rate law, with an observed rate constant that fits with established scattering-theory estimates for elementary two-body dissociative recombination. A small residual increase in this rate constant with decreasing charged-particle density suggests a growing importance of the three-body recombination channel under conditions of decreasing electron correlation.

DOI
10.1039/c1cp22624j

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Using state-selected double-resonant excitation, we create a Rydberg gas of NO molecules excited to the principal quantum number n = 50 of the f-series converging to the ion rotational level, N(+) = 2. This gas evolves to form an ultracold plasma, which expands under the thermal pressure of its electrons, and dissipates by electron-ion recombination. Under conditions chosen for this experiment, the observed rates of expansion vary with selected plasma density. Electron temperatures derived from these expansion rates vary from T(e) = 12 K for the highest density up to 16 K at four-fold lower density. Over this range, the apparent electron coupling parameter, defined as Γ(e) = e(2)/4πε(0)ak(B)T(e), falls from nearly three to about one. The decay of charged-particle density fits with a kinetic model that includes parallel paths of direct two-body and stepwise three-body dissociative recombination. The overall recombinative decay follows a second-order rate law, with an observed rate constant that fits with established scattering-theory estimates for elementary two-body dissociative recombination. A small residual increase in this rate constant with decreasing charged-particle density suggests a growing importance of the three-body recombination channel under conditions of decreasing electron correlation.
Double-resonant photoexcitation of nitric oxide in a molecular beam creates a dense ensemble of 50f(2) Rydberg states, which evolves to form a plasma of free electrons trapped in the potential well of an NO + space charge. The plasma travels at the velocity of the molecular beam and, on passing through a grounded grid, yields an electron time-of-flight signal that gauges the plasma size and quantity of trapped electrons. This plasma expands at a rate that fits with an electron temperature as low as 5 K, colder than typically observed for atomic ultracold plasmas. The recombination of molecular NO + cations with electrons forms neutral molecules excited by more than twice the energy of the NO chemical bond, and the question arises whether neutral fragmentation plays a role in shaping the redistribution of energy and particle density that directs the short-time evolution from Rydberg gas to plasma. To explore this question, we adapt a coupled rate-equations model established for atomic ultracold plasmas to describe the energy-grained avalanche of electron–Rydberg and electron–ion collisions in our system. Adding channels of Rydberg predissociation and two-body, electron–cation dissociative recombination to the atomic formalism, we investigate the kinetics by which this relaxation distributes particle density and energy over Rydberg states, free electrons and neutral fragments. The results of this investigation point to conditions under which such processes can effect the steady-state temperature of plasma electrons.
Double-resonant photoexcitation of nitric oxide in a molecular beam creates a dense ensemble of 51f(2) Rydberg states, which evolves to form a plasma of free electrons trapped in the potential well of an NO + spacecharge. The plasma travels at the velocity of the molecular beam, and, on passing through a grounded grid, yields an electron time-of-flight signal that gauges the plasma size and quantity of trapped electrons. This plasma expands at a rate that fits with an electron temperature as low as 5 K. Dissociative recombination of NO + ions with electrons provides the primary dissipation mechanism for the plasma. We have identified three dissociation pathways, and quantified their relative contributions to the measured rate: Two-body dissociative recombination competes with direct three-body recombination to neutral dissociation products, and with a process in which three-body recombination and electron-impact ionization form an equilibrium population of high-Rydberg states that decays by predissociation. Using available collision-theory rate constants for three-body recombination and ionization, together with quantum mechanical estimates of predissociation rates, we predict that the relaxation of the plasma to a high-Rydberg equilibrium outpaces direct three-body dissociative recombination, and, among second-order processes, the rate of two-body electron-cation dissociative recombination substantially exceeds the rate at which the high-Rydberg equilibrium dissociatively relaxes. The rate constant for dissociative recombination extracted from these data conforms with predictions drawn from theory for isolated electron-ion collisions. Methods based on the dissipation of molecular ultracold plasmas may provide a means for estimating rates of dissociative recombination for a variety of complex molecules.
We present a kinetic model based on coupled rate-equation simulations that accounts for state-detailed rate processes in the evolution of a molecular Rydberg gas to plasma. Calculations support a steady-state picture of Rydberg predissociation and its contribution to plasma dissipation. Inelastic collisions of electrons with Rydberg states efficiently transfer energy from and to the thermal bath of free electrons, giving rise to quasi equilibria of relatively high temperature. Dissipative effects that remove low- n population change the time course of this heating. Including statistically sampled channels of Rydberg predissociation with n - and ℓ-dependent lifetimes slows the relaxation to quasi equilibrium and retards the initial electron temperature increase. At later times, the dissociative loss of low- n population displaces this quasi equilibrium leading to continuous electron heating. Dissociation products appear at a rate that is controlled initially by the rate of Rydberg relaxation to quasi equilibrium. Thereafter, the overall rate at which the total dissociation consumes neutral molecules determines the decay rate for all levels. Simulations predict a total predissociation rate that is smaller than the initial rate of direct electron–ion dissociative recombination. At later times, residual predissociation displays an apparent first-order decay with a rate constant that fits well with experimental observations.
A fluid model for the expansion of a molecular ultracold plasma composed of NO+{}^{+}+ ions and electrons shows that fast dissociative recombination (DR) flattens the charged-particle density distribution, effectively freezing the expansion of the plasma core. However, a much greater fraction of the plasma mass exists at lower density in the wings of the plasma, where dissociative recombination has little effect, and ion motion is driven by a Gaussian charge-density gradient. Here, expansion proceeds as the collisionless acceleration of the ions under the radial pressure of the expanding electron gas. Even though DR flattening dramatically suppresses the radial velocity of ions in the densest part of the plasma, the measured evolution of the overall plasma width remains dominated by the expansion of the outer shells. Thus, despite its frozen core, a dissociating plasma with an initial electron temperature Te(0){T}_{e}(0)Te​(0) exhibits a time-evolving width that differs only slightly from a Vlasov expansion with the same Te(0){T}_{e}(0)Te​(0).
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.
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.