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Ultracold nitric oxide molecular plasma : characteristic response to time-varying electric fields

Seyed Mahyad Aghigh

Published Jan 1, 2021• 0 citations
Publisher

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 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.

DOI
10.14288/1.0396418

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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.
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.
Ultracold molecular plasmas represent a new frontier of plasma physics. They offer an easy and accessible laboratory for the study of strongly coupled Coulomb systems. Strong Coulomb coupling can give rise to exotic materials such as Wigner crystals and liquid like plasmas. In this thesis, I present a set of experiments and theoretical models that explore the properties of ultracold plasma in great detail. A supersonic beam of nitric oxide in helium creates a cold ensemble of ground state molecules. Upon two-color excitation, a Rydberg gas of nitric oxide evolves on a time scale of nanoseconds to form an ultracold plasma. The excited volume is imaged using a multichannel plate detector mounted on a movable grid. By moving the detector back and forth, we can observe the expansion dynamics of the plasma and its decay. Selective field ionization captures the relaxation of the Rydberg states to a plasma. We use a very reliable coupled-rate-equation model to understand the decay dynamics and evolution of Rydberg gas to a plasma by accounting for all the major processes that happen during the avalanche process. We find that a plasma evolved from an ultracold Rydberg gas expands very slowly, exhibits long relaxation time, and shows evidence suggesting the development of spatial order.
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.
Spontaneous avalanche to plasma begins in the core of an ellipsoidal Rydberg gas of nitric oxide. Ambipolar expansion of NO +^++ draws energy from avalanche-heated electrons. Then, cycles of long-range resonant electron transfer from Rydberg molecules to ions equalize their relative velocities. This sequence of steps gives rise to a remarkable mechanics of self-assembly, in which the kinetic energy of initially formed hot electrons and ions drives an observed separation of plasma volumes. These dynamics adiabatically sequester energy in a reservoir of mass transport, starting a process that anneals separating volumes to form an apparent glass of strongly coupled ions and electrons. Short-time electron spectroscopy provides experimental evidence for complete ionization. The long lifetime of this system, particularly its stability with respect to recombination and neutral dissociation, suggests that this transformation affords a robust state of arrested relaxation, far from thermal equilibrium. We see this most directly in the excitation spectrum of transitions to states in the initially selected Rydberg series, detected as the long-lived signal that survives a flight time of 500 μ500\ \mathrm {\mu }500 μ s to reach an imaging detector. The initial density of electrons produced by prompt Penning ionization, which varies with the selected initial principal quantum number and density of the Rydberg gas, determines a balance between the rising density of ions and the falling density of Rydberg molecules. This Penning-regulated ion-Rydberg molecule balance appears necessary as a critical factor in achieving the long ultracold plasma lifetime to produce spectral features detected after very long delays.
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.