On the formation and decay of a molecular ultracold plasma

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$^+$ 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, colder that 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 suggest some mechanisms by which molecular fragmentation channels can affect the state of the plasma

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

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

Delocalized excitons and interaction effects in extremely dilute thermal ensembles

Long-range interparticle interactions are revealed in extremely dilute thermal atomic ensembles using highly sensitive nonlinear femtosecond spectroscopy. Delocalized excitons are detected in the atomic systems at particle densities where the mean interatomic distance (410 mm) is much greater than the laser wavelength and multi-particle coherences should destructively interfere over the ensemble average. With a combined experimental and theoretical analysis, we identify an effective interaction mechanism, presumably of dipolar nature, as the origin of the excitonic signals. Our study implies that even in highly-dilute thermal atom ensembles, significant transition dipole-dipole interaction networks may form that require advanced modeling beyond the nearest neighbor approximation to quantitatively capture the details of their many-body properties

Dissociative recombination and the decay of a molecular ultracold 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

Dissociation and the development of spatial correlation in a molecular ultracold plasma.

Penning ionization initiates the evolution of a dense molecular Rydberg gas to plasma. This process selects for pairs of excited molecules separated by a distance of two Rydberg orbital diameters or less. The deactivated Penning partners predissociate, depleting the leading edge of the distribution of nearest-neighbor distances. For certain density and orbital radii, this sequence of events can form a plasma in which large distances separate a disproportionate fraction of the ions. Experimental results and model calculations suggest that the reduced potential energy of this Penning lattice significantly affects the development of strong coupling in an ultracold plasma

Dissociation and the development of spatial correlation in a molecular ultracold plasma.

Penning ionization initiates the evolution of a dense molecular Rydberg gas to plasma. This process selects for pairs of excited molecules separated by a distance of two Rydberg orbital diameters or less. The deactivated Penning partners predissociate, depleting the leading edge of the distribution of nearest-neighbor distances. For certain density and orbital radii, this sequence of events can form a plasma in which large distances separate a disproportionate fraction of the ions. Experimental results and model calculations suggest that the reduced potential energy of this Penning lattice significantly affects the development of strong coupling in an ultracold plasma