The energy-resolved rate coefficient for the dissociative recombination (DR) of H(3)(+) with slow electrons has been measured by the storage-ring method using an ion beam produced from a radiofrequency multipole ion trap, employing buffer-gas cooling at 13 K. The electron energy spread of the merged-beams measurement is reduced to 500 microeV by using a cryogenic GaAs photocathode. This and a previous cold- measurement jointly confirm the capability of ion storage rings, with suitable ion sources, to store and investigate H(3)(+) in the two lowest, (J,G) = (1,1) and (1,0) rotational states prevailing also in cold interstellar matter. The use of para-H(2) in the ion source, expected to enhance para-H(3)(+) in the stored ion beam, is found to increase the DR rate coefficient at meV electron energies.
The destruction of CH + ions in collisions with H atoms has been studied in a temperature-variable 22 pole ion trap (22PT) combined with a cold effusive H-atom beam. The stored ions are relaxed to temperatures of T 22PT 12 K. The hydrogen atoms, produced in a radio frequency discharge, are slowed down to various temperatures of T ACC 7 K. They are formed into an effusive beam. The effective density of the hydrogen atoms in the trap as well as the H 2 background are determined in situ using chemical probing with CO 2 +. The experimental arrangement allows us not only to measure thermal rate coefficients (T 22PT = T ACC), but also to extract state-specific rate coefficients k(J,T t) at selected translational temperatures T t and for the CH + rotational states J = 0, 1, and 2. The measured thermal rate coefficients have a maximum at 60 K, k = (1.2 ± 0.5)×10 −9 cm 3 s −1. Toward higher temperatures, they fall off in accordance with previous measurements and the trend predicted by phase space theory. Toward lower temperatures, the rate coefficients decrease significantly, especially if the rotation of the ions is cooled. At the coldest conditions achieved (beam: 7.3 K; trap: 12.2 K), a value as low as (5 ± 4) × 10 −11 cm 3 s −1 has been measured. This leads to the conclusion that non-rotating CH + is protected against attacks of H atoms. This surprising result is not yet understood. It is most probably due to quantum-dynamical effects already occurring at large distances.
We study binary and the recently discovered process of ternary He-assisted recombination of H 3 + ions with electrons in a low-temperature afterglow plasma. The experiments are carried out over a broad range of pressures and temperatures of an afterglow plasma in a helium buffer gas. Binary and He-assisted ternary recombination are observed and the corresponding recombination rate coefficients are extracted for temperatures from 77 to 330 K. We describe the observed ternary recombination as a two-step mechanism: first, a rotationally excited long-lived neutral molecule H 3 ء is formed in electron-H 3 + collisions. Second, the H 3 ء molecule collides with a helium atom that leads to the formation of a very long-lived Rydberg state with high orbital momentum. We present calculations of the lifetimes of H 3 ء and of the ternary recombination rate coefficients for para-and ortho-H 3 + . The calculations show a large difference between the ternary recombination rate coefficients of ortho-and para-H 3 + at temperatures below 300 K. The measured binary and ternary rate coefficients are in reasonable agreement with the calculated values.
Infrared absorption spectroscopy of few hundred H+(3) ions trapped in a 22-pole ion trap is presented using chemical probing as a sensitive detection technique down to the single ion level. By exciting selected overtone transitions of the (v(1)=0,v(2) (l)=3(1))<--(0,0(0)) vibrational band using an external cavity diode laser an accurate diagnostics measurement of the effective translational and rotational temperatures of the trapped ions was performed. The absolute accuracy of the measured transition frequencies was improved by a factor of four compared to previous plasma spectroscopy measurements using velocity modulation [Ventrudo et al., J. Chem. Phys. 100, 6263 (1994)]. The observed buffer gas cooling conditions in the ion trap indicate how to cool trapped H+(3) ions into the lowest ortho and para rotational states. Future experiments will utilize such an internally cold ion ensemble for state-selected dissociative recombination experiments at the heavy ion storage ring Test Storage Ring (TSR).
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