Experimental studies of ion-neutral reactions under astrophysical conditions

Ion-neutral collisions are pivotal for the gas-phase synthesis of complex molecules in the interstellar medium. Accurate modeling of the astrochemical network relies on precise laboratory data of reaction rate coefficients and their branching ratios. For the majority of ion-neutral reactions, rate coefficients at astrophysical conditions are completely unknown. To gain an experimental insight of ion-neutral, gas-phase chemistry under interstellar conditions, two different experimental approaches are presented. One of the most fundamental ions for interstellar chemistry is H3+ . This ion is assumed to be thermalized in collisions with H2. However, recent astronomical observations of H2 and H3+ in diffuse interstellar clouds revealed a significant difference in their excitation temperatures. In this work, 22 pole trap measurements, performed at the Max Planck Institute for Nuclear Physics (MPIK) in Heidelberg, of the H3++ H2 reaction at thermal equilibrium are presented and discussed. For future experiments on ion-atom reactions, an injection beamline for the Cyrogenic Storage Ring (CSR) was developed to perform merged-beams experiments on neutral ground-state atoms superimposed with the cooled, stored ions in the CSR

Generation of neutral atomic beams utilizing photodetachment by high power diode laser stacks

We demonstrate the use of high power diode laser stacks to photodetach fast hydrogen and carbon anions and produce ground term neutral atomic beams. We achieve photodetachment efficiencies of $\sim$7.4\% for H$^-$ at a beam energy of 10\,keV and $\sim$3.7\% for C$^-$ at 28\,keV. The diode laser systems used here operate at 975\,nm and 808\,nm, respectively, and provide high continuous power levels of up to 2\,kW, without the need of additional enhancements like optical cavities. The alignment of the beams is straightforward and operation at constant power levels is very stable, while maintenance is minimal. We present a dedicated photodetachment setup that is suitable to efficiently neutralize the majority of stable negative ions in the periodic table

Radiative rotational lifetimes and state-resolved relative detachment cross sections from photodetachment thermometry of molecular anions in a cryogenic storage ring

Photodetachment thermometry on a beam of OH$^-$ in a cryogenic storage ring cooled to below 10 K is carried out using two-dimensional, frequency and time dependent photodetachment spectroscopy over 20 minutes of ion storage. In equilibrium with the low-level blackbody field, we find an effective radiative temperature near 15 K with about 90% of all ions in the rotational ground state. We measure the J = 1 natural lifetime (about 193 s) and determine the OH$^-$ rotational transition dipole moment with 1.5% uncertainty. We also measure rotationally dependent relative near-threshold photodetachment cross sections for photodetachment thermometry.Comment: Manuscript LaTeX with 5 pages, 3 figures, and 1 table plus LaTeX supplement with 12 pages, 3 figures and 3 tables. This article has been accepted by Physical Review Letter

Experimental Determination of the Dissociative Recombination Rate Coefficient for Rotationally Cold CH⁺ and Its Implications for Diffuse Cloud Chemistry

Observations of CH+ are used to trace the physical properties of diffuse clouds, but this requires an accurate understanding of the underlying CH+ chemistry. Until this work, the most uncertain reaction in that chemistry was dissociative recombination (DR) of CH+. Using an electron–ion merged-beams experiment at the Cryogenic Storage Ring, we have determined the DR rate coefficient of the CH+ electronic, vibrational, and rotational ground state applicable for different diffuse cloud conditions. Our results reduce the previously unrecognized order-of-magnitude uncertainty in the CH+ DR rate coefficient to ∼20% and are applicable at all temperatures relevant to diffuse clouds, ranging from quiescent gas to gas locally heated by processes such as shocks and turbulence. Based on a simple chemical network, we find that DR can be an important destruction mechanism at temperatures relevant to quiescent gas. As the temperature increases locally, DR can continue to be important up to temperatures of ∼600 K, if there is also a corresponding increase in the electron fraction of the gas. Our new CH+ DR rate-coefficient data will increase the reliability of future studies of diffuse cloud physical properties via CH+ abundance observations

Astrochemistry in an Ion Storage Ring

Storage ring studies of low energy electron collisions with molecular ions have been carried out for dissociative recombination (DR) of fluorine-bearing molecules. Here we report on work aiming to improve the understanding of astrochemistry involving HF, a possible spectroscopic tracer of interstellar H2. For CF+ the rate coefficient was obtained for temperatures down to 10 K. For D2F+ the DR fragmentation branching ratios were determined to be 66(3)%, 24(2)%, and 10(2)% for the F+D+D, DF+D, and D2+F channels, respectively. The molecular DR products of this reaction, DF and D2, display an unusually high level of internal excitation, close to their dissociation limit

Dissociative recombination measurements of NH+ using an ion storage ring

We have investigated dissociative recombination (DR) of NH+ with electrons using a merged beams configuration at the TSR heavy-ion storage ring located at the Max Planck Institute for Nuclear Physics in Heidelberg, Germany. We present our measured absolute merged-beams recombination rate coefficient for collision energies from 0 to 12 eV. From these data, we have extracted a cross section, which we have transformed to a plasma rate coefficient for the collisional plasma temperature range from T pl = 10 to 18,000 K. We show that the NH+ DR rate coefficient data in current astrochemical models are underestimated by up to a factor of approximately nine. Our new data will result in predicted NH+ abundances lower than those calculated by present models. This is in agreement with the sensitivity limits of all observations attempting to detect NH+ in interstellar clouds

Exploring high-energy doubly excited states of NH by dissociative recombination of NH+

We have investigated electron capture by NH+ resulting in dissociative recombination (DR). The impact energies studied of ~4–12 eV extend over the range below the two lowest predicted NH+ dissociative states in the Franck–Condon (FC) region of the ion. Our focus has been on the final state populations of the resulting N and H atoms. The neutral DR fragments are detected downstream of a merged electron and ion beam interaction zone in the TSR storage ring, which is located at the Max Planck Institute for Nuclear Physics in Heidelberg, Germany. Transverse fragment distances were measured on a recently developed high count-rate imaging detector. The distance distributions enabled a detailed tracking of the final state populations as a function of the electron collision energy. These can be correlated with doubly excited neutral states in the FC region of the ion. At low electron energy of ~5 eV, the atomic product final levels are nitrogen Rydberg states together with ground-state hydrogen. In a small electron energy interval near 7 eV, a significant part of the final state population forms hydrogen Rydberg atoms with nitrogen atoms in the first excited ($\rm ^2D$) term, showing the effect of Rydberg doubly excited states below the predicted 2 2Π ionic potential. The distance distributions above ~10 eV are compatible with nitrogen Rydberg states correlating to the doubly excited Rydberg state manifold below the ionic 2 4Σ− level

An ion-atom merged beams setup at the Cryogenic Storage Ring.

We describe a merged beams experiment to study ion-neutral collisions at the Cryogenic Storage Ring of the Max Planck Institute for Nuclear Physics in Heidelberg, Germany. We produce fast beams of neutral atoms in their ground term at kinetic energies between 10 and 300 keV by laser photodetachment of negative ions. The neutral atoms are injected along one of the straight sections of the storage ring, where they can react with stored molecular ions. Several dedicated detectors have been installed to detect charged reaction products of various product-to-reactant mass ranges. The relative collision energy can be tuned by changing the kinetic energy of the neutral beam in an independent drift tube. We give a detailed description of the setup and its capabilities, and present proof-of-principle measurements on the reaction of neutral C atoms with D ions