Near-infrared photoabsorption by C(60) dianions in a storage ring

We present a detailed study of the electronic structure and the stability of C(60) dianions in the gas phase. Monoanions were extracted from a plasma source and converted to dianions by electron transfer in a Na vapor cell. The dianions were then stored in an electrostatic ring, and their near-infrared absorption spectrum was measured by observation of laser induced electron detachment. From the time dependence of the detachment after photon absorption, we conclude that the reaction has contributions from both direct electron tunneling to the continuum and vibrationally assisted tunneling after internal conversion. This implies that the height of the Coulomb barrier confining the attached electrons is at least similar to 1.5 eV. For C(60)(2-) ions in solution electron spin resonance measurements have indicated a singlet ground state, and from the similarity of the absorption spectra we conclude that also the ground state of isolated C(60)(2-) ions is singlet. The observed spectrum corresponds to an electronic transition from a t(1u) lowest unoccupied molecular orbital (LUMO) of C(60) to the t(1g) LUMO+1 level. The electronic levels of the dianion are split due to Jahn-Teller coupling to quadrupole deformations of the molecule, and a main absorption band at 10723 cm(-1) corresponds to a transition between the Jahn-Teller ground states. Also transitions from pseudorotational states with 200 cm(-1) and (probably) 420 cm(-1) excitation are observed. We argue that a very broad absorption band from about 11 500 cm(-1) to 13 500 cm(-1) consists of transitions to so-called cone states, which are Jahn-Teller states on a higher potential-energy surface, stabilized by a pseudorotational angular momentum barrier. A previously observed, high-lying absorption band for C(60)(-) may also be a transition to a cone state

Lifetimes of C-60(2-) and C-70(2-) dianions in a storage ring

C-60(2-) and C-70(2-) dianions have been produced by electrospray of the monoanions and subsequent electron pickup in a Na vapor cell. The dianions were stored in an electrostatic ring and their decay by electron emission was measured up to 1 s after injection. While C-70(2-) ions are stable on this time scale, except for a small fraction of the ions which have been excited by gas collisions, most of the C-60(2-) ions decay on a millisecond time scale, with a lifetime depending strongly on their internal temperature. The results can be modeled as decay by electron tunneling through a Coulomb barrier, mainly from thermally populated triplet states about 120 meV above a singlet ground state. At times longer than about 100 ms, the absorption of blackbody radiation plays an important role for the decay of initially cold ions. The tunneling rates obtained from the modeling, combined with WKB estimates of the barrier penetration, give a ground-state energy 200 +/- 30 meV above the energy of the monoanion plus a free electron and a ground-state lifetime of the order of 20 s. (c) 2006 American Institute of Physics

Collisions of low-energy antiprotons with molecular hydrogen: ionization, excitation and stopping power

A time-dependent coupled-channel approach was used to calculate ionization, excitation, and energy-loss cross sections as well as energy spectra for antiproton and proton collisions with molecular hydrogen for impact energies 8 keV < E < 4000 keV.Comment: 4 pages, 4 figures, conference LEAP0

Close-coupling approach to antiproton-impact ionisation of H2 with analytical spherical averaging

Integrated cross section for single ionisation of molecular hydrogen by antiproton impact has been calculated in a wide range of impact energies from 1 keV up to 2 MeV using a close-coupling approach. For the first time all possible orientations of the molecular target have been accounted for using an ab initio analytical spherical averaging technique. Obtained results are in good agreement with experiment

Correlated Two Electron Effects in Collisions of Multiply Charged Au Ions with He

We have studied the fate of electrons released in collisions between highly charged Au/sup q+/ ions (20 MeV) and He atoms and find that the large transfer ionization (TI) cross section observed can be accounted for by transfer of two electrons to a highly correlated state on the Au projectile followed by the loss of one electron to the continuum. Autoionization lines are also observed, but they are attributable to electron transfer accompanied by core excitation (TE)

Ionization of hydrogen and hydrogenic ions by antiprotons

Presented here is a description of the ionization of hydrogen and hydrogenic ions by antiproton-impact, based on very large scale numerical solutions of the time-dependent Schr\"odinger equation in three spatial dimensions and on analysis of the topology of the electronic eigenenergy surfaces in the plane of complex internuclear distance. Comparison is made with other theories and very recent measurements.Comment: RevTex document, 11 pages, 4 Postscript figures are available from the authors, in press Phys. Rev. Let

Fully quantum-mechanical treatment of proton-hydrogen scattering

© Published under licence by IOP Publishing Ltd. A fully quantum-mechanical convergent close-coupling approach to proton collisions with atomic hydrogen has been developed. Cross sections for target ionisation and electron capture by the projectile have been calculated in the energy range from 20 keV to 1 MeV. Calculated electron capture cross sections are in good agreement with the experiment, however for ionisation discrepancies between theory and experiment at intermediate energies still remain

Stabilities of protonated water-ammonia clusters

Branching ratios of water and ammonia evaporation have been measured for spontaneous evaporation from protonated mixed clusters H + (H 2 O) n (NH 3 ) m in the size range 0 ≤ n ≤ 11 and 0 ≤ m ≤ 7. Mixed clusters evaporate water except for clusters containing six or more ammonia molecules, indicating the formation of a stable core of one ammonium ion surrounded by four ammonia molecules and a second shell consisting predominantly of water. We relate evaporative branching ratios to free energy differences between the products of competing channels and determine the free energy differences for clusters with up to seven ammonia molecules. Clusters containing up to five ammonia molecules show a very strong scaling of these free energy differences