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arXiv:0911.0466

Charge, density and electron temperature in a molecular ultracold plasma

Chris Rennick, J. P. Morrison, Jaime Ortega Arroyo, Paul J. Godin, Nicolas Saquet, Edward R. Grant

Published Nov 3, 2009• 1 citation
arXivHTMLPDF

Abstract

A Rydberg gas of NO entrained in a supersonic molecular beam releases electrons as it evolves to form an ultracold plasma. The size of this signal, compared with that extracted by the subsequent application of a pulsed electric field, determines the absolute magnitude of the plasma charge. This information, combined with the number density of ions, supports a simple thermochemical model that explains the evolution of the plasma to an ultracold electron temperature.

DOI
10.48550/arxiv.0911.0466

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A Rydberg gas of NO entrained in a supersonic molecular beam releases electrons as it evolves to form an ultracold plasma. The size of this signal, compared with that extracted by the subsequent application of a pulsed electric field, determines the absolute magnitude of the plasma charge. This information, combined with the number density of ions, supports a simple thermochemical model that explains the evolution of the plasma to an ultracold electron temperature.
Not long after metastable xenon was photoionized in a magneto-optical trap, groups in Europe and North America found that similar states of ionized gas evolved spontaneously from state-selected Rydberg gases of high principal quantum number. Studies of atomic xenon and molecular nitric oxide entrained in a supersonically cooled molecular beam subsequently showed much the same final state evolved from a sequence of prompt Penning ionization and electron impact avalanche to plasma, well-described by coupled rate-equation simulations. However, measured over longer times, the molecular ultracold plasma (UCP) was found to exhibit an anomalous combination of very long lifetime and very low apparent electron temperature. In this thesis I summarize early developments in the study of UCP formed by atomic and molecular Rydberg gases, and then I detail observations as they combine to characterize properties of the nitric oxide molecular UCP that appear to call for an explanation beyond the realm of conventional plasma physics. I also explain how I leveraged a radio frequency electric field to understand the causes of classically-unexplainable behavior of our molecular system.
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.
Abstract Not long after metastable xenon was photoionized in a magneto-optical trap, groups in Europe and North America found that similar states of ionized gas evolved spontaneously from state-selected, high principal quantum number Rydberg gases. Studies of atomic xenon and molecular nitric oxide entrained in a supersonically cooled molecular beam subsequently showed much the same final state evolved from a sequence of prompt Penning ionization and electron-impact avalanche to plasma, well-described by coupled rate-equation simulations. But, measured over longer times, the molecular ultracold plasma was found to exhibit an anomalous combination of very long lifetime and very low apparent electron temperature. This review first summarizes early developments in the general study of ultracold plasmas formed by atomic and molecular Rydberg gases, and then turns to describe the particular properties of the nitric oxide molecular ultracold plasma that appear to call for an explanation beyond the realm of conventional plasma physics.
A Rydberg gas of xenon, entrained in a supersonic atomic beam, evolves slowly to form an ultracold plasma. In the early stages of this evolution, when the free-electron density is low, Rydberg atoms undergo long-range -mixing collisions, yielding states of high orbital angular momentum. The development of high- states promotes dipole–dipole interactions that help to drive Penning ionization. The electron density increases until it reaches the threshold for avalanche. Ninety μs after the production of a Rydberg gas with the initial state, , a 432 V cm−1 electrostatic pulse fails to separate charge in the excited volume, an effect which is ascribed to screening by free electrons. Photoexcitation cross sections, observed rates of -mixing, and a coupled-rate-equation model simulating the onset of the electron-impact avalanche point consistently to an initial Rydberg gas density of .
Ultracold neutral plasmas (UNPs) are highly correlated, charged-particle systems studied in standard atomic-molecular optical physics laboratories. Advances in ultracold physics techniques have led to the development of magneto-optical traps that permit the localization of micro-Kelvin temperature atomic samples (10⁸ - 10¹⁰ cm -³ that can be photoionized with a defined excess laser energy. Magneto-optical trapping of molecules proves difficult, and to date, lags in reaching conditions attainable for atoms. Molecules possess additional degrees of freedom where energy can flow during laser trapping and cooling. Alternatively, elastic collisions with inert gases offer another route to low temperatures. Super-sonic expansions of target molecules seeded in a noble gas can reduced the translational temperature to values as low as 0.1 K. Here I report on the formation of a molecular ultracold plasma in a molecular beam of nitric oxide seeded in an inert gas. Our method does not directly form a plasma, but instead, I create a Rydberg gas that spontaneously evolves to a plasma. I have verified the transition to a collective plasma state by applying pulsed-fields to the field-free flight region, and observe a signal that persists well beyond classical field amplitudes required to ionize individual Rydberg states. Electric field screening is a collective effect occurring over a characteristic distance, quantified by the Debye length, λ_D. Molecular ultracold plasmas described here exhibit Debye lengths smaller than the overall size, λ_D<<σ. Plasmas of this nature offer an exotic environment for which to study fundamental phenomena. While plasmas are generally thought of as hot, UNPs exist at low enough temperatures that electrostatic interaction energy between particles is greater than their kinetic energy. At this point, charged particles begin to find themselves in local potential energy minima. Over the entire sample this translates to long-range order, or correlation. It is of great interest for researchers studying UNPs to maximize particle correlation, which requires UNPs to remain very cold, and dense through their lifetime.
The double-resonant laser excitation of nitric oxide, cooled to 1 K in a seeded supersonic molecular beam, yields a gas of $\ensuremath{\approx}{10}^{12}$ molecules per cubic centimeter in a single selected Rydberg state. This population evolves to produce prompt free electrons, and a durable cold plasma of electrons and intact NO+{\text{NO}}^{+}NO+ ions. This plasma travels with the molecular beam through a field-free region to encounter a grid. The atomic weight of the expansion gas controls the beam velocity and hence the flight time from the interaction region to the grid. Monitoring electron production as the plasma traverses this grid measures its longitudinal width as a function of flight time. Comparing these widths to the width of the laser beam that defines the initial size of the illuminated volume allows us to gauge the rate of expansion of the plasma. We find that the plasma created from the evolution of a Rydberg gas of NO expands at a small but measurable rate, and that this rate of expansion accords with the Vlasov equations for an initial electron temperature of ${T}_{e}\ensuremath{\approx}7\text{ }\text{K}$.