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arXiv:0812.4051 · Physical Review A

Very slow expansion of an ultracold plasma formed in a seeded supersonic molecular beam of NO

J. P. Morrison, Chris Rennick, Edward R. Grant

Published Jun 9, 2009• 29 citations
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Abstract

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 ${\text{NO}}^{+}$ 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 ${T}_{e}\ensuremath{\approx}7\text{ }\text{K}$.

DOI
10.1103/physreva.79.062706

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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.

•Jan 1, 2013•0 citations
The double-resonant laser excitation of nitric oxide, cooled to 1 K in a seeded supersonic molecular beam, yields a gas of \ensuremath≈1012\ensuremath{\approx}{10}^{12}\ensuremath≈1012 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 Te\ensuremath≈7 K{T}_{e}\ensuremath{\approx}7\text{ }\text{K}Te​\ensuremath≈7 K.
We report the spontaneous formation of a plasma from a gas of cold Rydberg molecules. Double-resonant laser excitation promotes nitric oxide, cooled to 1 K in a seeded supersonic molecular beam, to single Rydberg states extending as deep as $80\text{ }\text{ }{\mathrm{cm}}^{\ensuremath{-}1}$ below the lowest ionization threshold. The density of excited molecules in the illuminated volume approaches $1\ifmmode\times\else\texttimes\fi{}{10}^{13}\text{ }\text{ }{\mathrm{cm}}^{\ensuremath{-}3}$. This population evolves to produce free electrons and a durable cold plasma of electrons and intact NO+{\mathrm{NO}}^{+}NO+ ions.
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 Double-resonant transitions excite nitric oxide in a seeded supersonic molecular beam, yielding a state-selected Rydberg gas that evolves to form an ultracold plasma. This plasma propagates in z with the molecular beam over a variable distance as great as 600 mm to strike an imaging detector, which records the charge distribution in the dimensions, x and y . The laser-crossed molecular beam excitation geometry convolutes an axial Gaussian distribution of NO about z with the Gaussian intensity distribution of the laser beam about x to create an ellipsoidal volume of Rydberg gas. Plasma images provide evidence for the relaxation of this Rydberg gas volume in an electron impact avalanche that breaks the ellipsoidal symmetry in x to form repelling plasma volumes. We find that the energy deposited in the recoil velocity of mass transport, V x depends systematically on the initially selected Rydberg gas principal quantum number, n 0 , and the initial density of the Rydberg gas, ρ 0 . These quantities combine to determine ρ e , the initial density of electrons formed by the prompt Penning ionization of closely spaced pairs of Rydberg molecules. Above a threshold density of Penning electrons, we find that V x depends linearly on ρ e . We argue that this bifurcation occurs as a consequence of the initial geometry of the Rydberg gas. Ambipolar electron expansion accelerates initially formed core ions. Resonant charge transfer redistributes this ion energy to the column of Rydberg molecules on the long axis of the ellipsoid. The equalized velocities in each direction give rise to a ± x streaming motion that concentrates density in opposing plasma volumes, causing the symmetric gas volume to split like a rotating liquid drop. Significantly, these dynamics reduce electron temperature with little decrease in the ion density or increase in the ion temperature. This appears to facilitate the formation of a strongly coupled plasma.
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.
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.