Measurements in H(3)(+) afterglow plasmas with spectroscopically determined relative abundances of H(3)(+) ions in the para-nuclear and ortho-nuclear spin states provide clear evidence that at low temperatures (77-200 K) para-H(3)(+) ions recombine significantly faster with electrons than ions in the ortho state, in agreement with a recent theoretical prediction. The cavity ring-down absorption spectroscopy used here provides an in situ determination of the para/ortho abundance ratio and yields additional information on the translational and rotational temperatures of the recombining ions. The results show that H(3)(+) recombination with electrons occurs by both binary recombination and third-body (helium) assisted recombination, and that both the two-body and three-body rate coefficients depend on the nuclear spin states. Electron-stabilized (collisional-radiative) recombination appears to make only a small contribution.
We have applied a continuous-wave near-infrared cavity ring-down spectroscopy method to study the parameters of a H + 3 -dominated plasma at temperatures in the range 77-200 K. We monitor populations of three rotational states of the ground vibrational state corresponding to para and ortho nuclear spin states in the discharge and the afterglow plasma in time and conclude that abundances of para and ortho states and rotational temperatures are well defined and stable. The non-trivial dependence of a relative population of para-H + 3 on a relative population of para-H 2 in a source H 2 gas is described. The results described in this paper are valuable for studies of state-selective dissociative recombination of H + 3 ions with electrons in the afterglow plasma and for the design of sources of H + 3 ions in a specific nuclear spin state.
We present results of plasma afterglow experiments on ternary electron-ion recombination rate coefficients of H3(+) and D3(+) ions at temperatures from 50 to 300 K and compare them to possible three-body reaction mechanisms. Resonant electron capture into H3* Rydberg states is likely to be the first step in the ternary recombination, rather than third-body-assisted capture. Subsequent interactions of the Rydberg molecules with ambient neutral and charged particles provide the rate-limiting step that completes the recombination. A semiquantitative model is proposed that reconciles several previously discrepant experimental observations. A rigorous treatment of the problem will require additional theoretical work and experimental investigations.
Ice nanoparticles (H2O)N, N ≈ 450 generated in a molecular beam experiment pick up individual gas phase molecules of 2-hydroxypyridine and 2-pyridone (HP) evaporated in a pickup cell at temperatures between 298 and 343 K. The mass spectra of the doped nanoparticles show evidence for generation of clusters of adsorbed molecules (HP)n up to n = 8. The clusters are ionized either by 70 eV electrons or by two photons at 315 nm (3.94 eV). The two ionization methods yield different spectra, and their comparison provides an insight into the neutral cluster composition, ionization and intracluster ion-molecule reactions, and cluster fragmentation. Quite a few molecules were reported not to coagulate on ice nanoparticles previously. The (HP)n cluster generation on ice nanoparticles represents the first evidence for coagulating of molecules and cluster formation on free ice nanoparticles. For comparison, we investigate the coagulation of HP molecules picked up on large clusters ArN, N ≈ 205, and also (HP)n clusters generated in supersonic expansions with Ar buffer gas. This comparison points to a propensity for the (HP)2 dimer generation on ice nanoparticles. This shows the feasibility of base pairing for model of biological molecules on free ice nanoparticles. This result is important for hypotheses of the biomolecule synthesis on ice grains in the space. We support our findings by theoretical calculations that show, among others, the HP dimer structures on water clusters.
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