M. Froese

A cryogenic electrostatic trap for long-time storage of keV ion beams

We report on the realization and operation of a fast ion beam trap of the linear electrostatic type employing liquid helium cooling to reach extremely low blackbody radiation temperature and residual gas density and, hence, long storage times of more than 5 min which are unprecedented for keV ion beams. Inside a beam pipe that can be cooled to temperatures <15 K, with 1.8 K reached in some locations, an ion beam pulse can be stored at kinetic energies of 2-20 keV between two electrostatic mirrors. Along with an overview of the cryogenic trap design, we present a measurement of the residual gas density inside the trap resulting in only 2 x 10(3) cm(-3), which for a room temperature environment corresponds to a pressure in the 10(-14) mbar range. The device, called the cryogenic trap for fast ion beams, is now being used to investigate molecules and clusters at low temperatures, but has also served as a design prototype for the cryogenic heavy-ion storage ring currently under construction at the Max-Planck Institute for Nuclear Physics.

COLD ELECTRON REACTIONS PRODUCING THE ENERGETIC ISOMER OF HYDROGEN CYANIDE IN INTERSTELLAR CLOUDS

Using event-by-event fragment momentum spectroscopy in a storage-ring merged-beams experiment, we find laboratory evidence that in the dissociative recombination (DR) of HCNH{sup +} with cold electrons the energetic isomer HNC is produced with a high yield, similar to that of HCN. With a newly implemented mass-sensitive fragment imaging detector, we analyze the kinetic energy release of the triatomic fragments DCN/DNC from the DR reaction of the isotopologue DCND{sup +} with cold (near 10 K) electrons. The results show that the internal energy of these fragments is extremely high, far exceeding the isomerization barrier between DNC and DCN. From this laboratory characterization of the DR reaction we conclude that also the triatomic fragment HCN/HNC from the DR of HCNH{sup +} will carry a large amount of ro-vibrational excitation and show that this implies an isomeric production ratio in a narrow range near unity.

The cryogenic storage ring CSR

An electrostatic cryogenic storage ring, CSR, for beams of anions and cations with up to 300 keV kinetic energy per unit charge has been designed, constructed, and put into operation. With a circumference of 35 m, the ion-beam vacuum chambers and all beam optics are in a cryostat and cooled by a closed-cycle liquid helium system. At temperatures as low as (5.5 ± 1) K inside the ring, storage time constants of several minutes up to almost an hour were observed for atomic and molecular, anion and cation beams at an energy of 60 keV. The ion-beam intensity, energy-dependent closed-orbit shifts (dispersion), and the focusing properties of the machine were studied by a system of capacitive pickups. The Schottky-noise spectrum of the stored ions revealed a broadening of the momentum distribution on a time scale of 1000 s. Photodetachment of stored anions was used in the beam lifetime measurements. The detachment rate by anion collisions with residual-gas molecules was found to be extremely low. A residual-gas density below 140 cm(-3) is derived, equivalent to a room-temperature pressure below 10(-14) mbar. Fast atomic, molecular, and cluster ion beams stored for long periods of time in a cryogenic environment will allow experiments on collision- and radiation-induced fragmentation processes of ions in known internal quantum states with merged and crossed photon and particle beams.

Fragmentation Channels in Dissociative Electron Recombination with Hydronium and Other Astrophysically Important Species

We report on our recent studies of dissociative recombination (DR) employing two different fragment imaging detection techniques at the TSR storage ring in Heidelberg, Germany. Principles of an upgraded 3D optical system and the new energy-sensitive multistrip detector (EMU) are explained together with possible applications in reaction dynamics studies. With the EMU imaging detector we succeeded to observe the branching ratios after DR of deuterated hydronium ions D(3)O(+) at energies of 0-0.5 and 4-21 eV. The branching ratios are almost constant at low energies while above 6 eV both oxygen-producing channels O + D + D + D and O + D(2) + D strongly increase and dominate by about 85% at 11 eV. To demonstrate further capabilities of our fragment imaging detectors, we also summarize some of our additional recent studies on DR of molecular ions important for astrophysics as well as for fundamental unimolecular dynamics.

Electron collisions and rovibrational action spectroscopy of cold H3+ molecules

Electron recombination of H3+ has found a lot of attention due to its outstanding relevance for the chemistry of the interstellar medium (ISM) and its role as a benchmark for the treatment of dissociative recombination (DR) of polyatomic ions. We report DR measurements performed at the TSR storage ring utilizing a cryogenic ion trap injector. Furthermore, a chemical probing spectroscopy technique is described that allows for a very sensitive monitoring of the populated states inside the ion injector. Since H3+ exists in two different nuclear spin modifications, a controlled manipulation of the ortho/para fraction is needed in order to perform state-selective measurements.

Spectroscopy and dissociative recombination of the lowest rotational states of H+3

The dissociative recombination of the lowest rotational states of H3+ has been investigated at the storage ring TSR using a cryogenic 22-pole radiofrequency ion trap as injector. The H3+ was cooled with buffer gas at ~15 K to the lowest rotational levels, (J, G)=(1,0) and (1,1), which belong to the ortho and para proton-spin symmetry, respectively. The rate coefficients and dissociation dynamics of H3+(J, G) populations produced with normal-and para-H2 were measured and compared to the rate and dynamics of a hot H3+ beam from a Penning source. The production of cold H3+ rotational populations was separately studied by rovibrational laser spectroscopy using chemical probing with argon around 55 K. First results indicate a ~20% relative increase of the para contribution when using para-H2 as parent gas. The H3+ rate coefficient observed for the para-H2 source gas, however, is quite similar to the H3+ rate for the normal-H2 source gas. The recombination dynamics confirm that for both source gases, only small populations of rotationally excited levels are present. The distribution of 3-body fragmentation geometries displays a broad part of various triangular shapes with an enhancement of ~12% for events with symmetric near-linear configurations. No large dependences on internal state or collision energy are found.

The Cryogenic Storage Ring and its application to molecular ion recombination physics

The Cryogenic Storage Ring (CSR), presently under construction at the Max-Planck-Institute for Nuclear Physics, will allow the storage of large ionic molecules under optimum experimental conditions. The electrostatic beam optics and the presence of a low-energy electron cooler will allow highly-precise recombination experiments with molecular ions of 160 atomic mass units per charge state. The all-cryogenic design of the storage ring will provide unprecedented vacuum conditions and assure long storage times even for very heavy ion beams. Suppression of the black body radiation background of the beam pipe in combination with electron cooling will give access to internal ion temperatures of 10K and allow state-selective experiments on infrared-active species, impossible in present-day room-temperature storage rings. We give an overview of the CSR project, point out the scientific opportunities arising from its unique design, and give an outlook on possible first molecular recombination experiments after commissioning of the storage ring.

Anisotropic fragmentation in low-energy dissociative recombination

On a dense energy grid reaching up to 75 meV electron collision energy the fragmentation angle and the kinetic energy release of neutral dissociative recombination fragments have been studied in a twin merged beam experiment. The anisotropy and the extracted rotational state contributions were found to sensitively depend on energy. Both show pronounced variations on a likewise narrow energy scale as the rotationally averaged rate coefficient. For the first time angular dependences described by Legendre polynomials higher than 2nd order could be deduced. Moreover, a slight anisotropy at zero collision energy was observed which is caused by the flattened velocity distribution of the electron beam.

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.

Fragmentation by electron recombination for HF+ and CF+

Dissociative recombination (DR) is an exothermic process leading to neutralisation and chemical fragmentation in many plasma environments, down to the lowest temperatures. We present results of complex investigations on DR of HF+ and CF+ performed at the TSR storage ring. Beyond the rate coefficient down to meV collision energies also dissociation pathways and geometries have been investigated using full 3D fragment imaging technique. Fragment imaging also provides HF+ rotational structure and fine-structure as well as the HF+ dissociation energy with sub-meV precision.