The energy dependence of the rates of the reactions between He+ and ammonia (NY3, Y = {H,D}), forming NY2+, Y and He as well as NY+, Y2 and He has been measured at low collision energies near 0 K.
Recently, a new method has been introduced to study ion-molecule reactions at very low collision energies, down to below k
B ⋅ 1 K (Allmendinger et al 2016 ChemPhysChem
17 3596). To eliminate the acceleration of the ions by stray electric fields in the reaction volume, the reactions are observed within the orbit of a Rydberg electron with large principal quantum number n > 20. This electron is assumed not to influence the reaction taking place between the ion core and the neutral molecules. This assumption is tested here with the example of the He(n) + CO → C(n′) + O + He reaction, which is expected to be equivalent to the He+ + CO → C+ + O + He reaction, using a merged-beam approach enabling measurements of relative reaction rates for collision energies E
coll in the range from 0 to about k
B ⋅ 25 K with a collision-energy resolution of ∼k
B ⋅ 200 mK at E
coll = 0. In contrast to the other ion-molecule reactions studied so far with this method, the atomic ion product (C+) is in its electronic ground state and does not have rotational and vibrational degrees of freedom so that the corresponding Rydberg product [C(n′)] cannot decay by autoionization. Consequently, one can investigate whether the principal quantum number is effectively conserved, as would be expected in the spectator Rydberg-electron model. We measure the distribution of principal quantum numbers of the reactant He(n) and product C(n′) Rydberg atoms by pulsed-field ionization following initial preparation of He(n) in states with n values between 30 and 45 and observe that the principal quantum number of the Rydberg electron is conserved during the reaction. This observation indicates that the Rydberg electron is not affected by the reaction, from which we can conclude that it does not affect the reaction either. This conclusion is strengthened by measurements of the collision-energy-dependent reaction yields at n = 30, 35 and 40, which exhibit the same behavior, i.e. a marked decrease below E
coll ≈ k
B ⋅ 5 K.
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 summarizes early developments in the study of ultracold plasmas formed by atomic and molecular Rydberg gases, and then details observations as they combine to characterize properties of the nitric oxide molecular ultracold plasma that appear to call for an explanation beyond the realm of conventional plasma physics.
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