We have experimentally investigated dissociative recombination of NH+ with electrons using a merged ion and electron beam configuration in a storage ring. A fast counting and position sensitive imaging detector enabled us to perform fragment imaging measurements over relative electron-ion collision energies from 0 to 12 eV. The results show unprecedented details on product excitation and on the reaction dynamics.
We have investigated electron capture by NH+ resulting in dissociative recombination (DR). The impact energies studied of similar to 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 similar to 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 (D-2) term, showing the effect of Rydberg doubly excited states below the predicted 2(2)Pi ionic potential. The distance distributions above similar to 10 eV are compatible with nitrogen Rydberg states correlating to the doubly excited Rydberg state manifold below the ionic 2(4) Sigma(-) level.
We have measured electron–ion recombination for C-like Mg6 + forming Mg5 +, and for B-like Mg7 + forming Mg6 +. These studies were performed using a merged electron–ion beam arrangement at the TSR heavy ion storage ring located in Heidelberg, Germany. Both primary ions have metastable levels with significant lifetimes. Using a simple cascade model we estimate the population fractions in these metastable levels. For the Mg6 + results, we find that the majority of the stored ions are in a metastable level, while for Mg7 + the metastable fraction is insignificant. We present the Mg6 + merged beams recombination rate coefficient for DR via N = 2 → N′ = 2 core electron excitations (ΔN = 0 DR) and for Mg7 + via 2 → 2 and 2 → 3 core excitations. Taking the estimated metastable populations into account, we compare our results to state-of-the-art multiconfiguration Breit–Pauli theoretical calculations. Significant differences are found at low energies where theory is known to be unreliable. Moreover, for both ions we observe a discrepancy between experiment and theory for ΔN = 0 DR involving capture into high-n Rydberg levels and where the stabilization is primarily due to a radiative transition of the excited core electron. This is consistent with previous DR experiments on M-shell iron ions which were performed at TSR. The large metastable content of the Mg6 + ion beam precludes generating a plasma recombination rate coefficient (PRRC). However, this is not an issue for Mg7 + and we present an experimentally derived Mg7 + PRRC for plasma temperatures from 400 K to 107 K with an estimated uncertainty of less than 27% at a 90% confidence level. We also provide a fit to our experimentally derived PRRC for use in plasma modeling codes.
We have measured electron-ion recombination for C-like Mg6+ forming Mg5+, and for B-like Mg7+ forming Mg6+. These studies were performed using a merged electron-ion beam arrangement at the TSR heavy ion storage ring located in Heidelberg, Germany. Both primary ions have metastable levels with significant lifetimes. Using a simple cascade model we estimate the population fractions in these metastable levels. For the Mg6+ results, we find that the majority of the stored ions are in a metastable level, while for Mg7+ the metastable fraction is insignificant. We present the Mg6+ merged beams recombination rate coefficient for DR via N = 2 -> N' = 2 core electron excitations (Delta N = 0 DR) and for Mg7+ via 2 -> 2 and 2 -> 3 core excitations. Taking the estimated metastable populations into account, we compare our results to state-of-the-art multiconfiguration Breit-Pauli theoretical calculations. Significant differences are found at low energies where theory is known to be unreliable. Moreover, for both ions we observe a discrepancy between experiment and theory for Delta N = 0 DR involving capture into high-n Rydberg levels and where the stabilization is primarily due to a radiative transition of the excited core electron. This is consistent with previous DR experiments on M-shell iron ions which were performed at TSR. The large metastable content of the Mg6+ ion beam precludes generating a plasma recombination rate coefficient (PRRC). However, this is not an issue for Mg7+ and we present an experimentally derived Mg7+ PRRC for plasma temperatures from 400 K to 107 K with an estimated uncertainty of less than 27% at a 90% confidence level. We also provide a fit to our experimentally derived PRRC for use in plasma modeling codes.
We have investigated the radiative cooling of initially hot Al−4 and Al−5 cluster anions during storage in a cryogenic ion beam trap at an ambient temperature of <15 K. By applying a statistical rate model to the ions' measured delayed detachment rate following excitation with a laser, we have obtained their vibrational temperature as a function of cooling time. The temperature curves for Al−4 suggest that the vibrational cooling slows down considerably once the ion reaches approximately room temperature. This suggests the participation of transitions from recently found low-lying electronic states of the anion in the cooling process, prior to reaching approximately room temperature. The experimental results for Al−5 suggest slightly slower radiative cooling than for Al−4.
In an article Missing Transverse-Doppler Effect in Time-Dilation Experiments with High-Speed Ions by S. Devasia [arXiv:1003.2970v1], our recent Doppler shift experiments on fast ion beams are reanalyzed. Contrary to our analysis, Devasia concludes that our results provide an indication of Lorentz violation. We argue that this conclusion is based on a fundamental misunderstanding of our experimental scheme and reiterate that our results are in excellent agreement with Special Relativity.
We present preparatory measurements for an improved test of time dilation at the experimental storage ring (ESR) at GSI in Darmstadt. A unique combination of particle accelerator experiments and laser spectroscopy is used to perform this test with the highest precision. Li-7(+) ions are accelerated to 34% of the speed of light at the GSI Helmholtz-zentrum fur Schwerionenforschung and stored in the experimental storage ring. The forward and backward Doppler shifts of an electric dipole transition of these ions are measured with laser spectroscopy techniques. From these Doppler shifts, both the ion velocity beta = nu/c and the time dilation factor gamma = gamma(SR)(1 + (alpha) over cap beta(2)) can be derived for testing Special Relativity. Two laser systems have been developed to drive the S-3(1)-> P-3(2) transition in Li-7(+). Moreover, a detector system composed of photomultipliers, both to monitor the exact laser ion beam overlap as well as to optimize fluorescence detection, has been set up and tested. We investigate optical-optical double-resonance spectroscopy on a closed L-type three-level system to overcome Doppler broadening. A residual, broadened fluorescence background caused by velocity-changing processes in the ion beam is identified, and a background subtraction scheme implemented. At the present stage the experimental sensitivity, although already comparable with previous measurements on slower ion beams at the TSR storage ring that led to vertical bar(alpha) over cap vertical bar < 8.4 x 10(-8), suffer from a poor signal-to-noise ratio. Modifications of the ion source as well as the detection system are discussed that promise to improve the sensitivity by one order of magnitude.
We present preparatory measurements for an improved test of time dilation at the experimental storage ring (ESR) at GSI in Darmstadt. A unique combination of particle accelerator experiments and laser spectroscopy is used to perform this test with the highest precision. 7Li+ ions are accelerated to 34% of the speed of light at the GSI Helmholtzzentrum für Schwerionenforschung and stored in the experimental storage ring. The forward and backward Doppler shifts of an electric dipole transition of these ions are measured with laser spectroscopy techniques. From these Doppler shifts, both the ion velocity β = ν/c and the time dilation factor [Formula: see text] can be derived for testing Special Relativity. Two laser systems have been developed to drive the 3S1→3P2 transition in 7Li+. Moreover, a detector system composed of photomultipliers, both to monitor the exact laser ion beam overlap as well as to optimize fluorescence detection, has been set up and tested. We investigate optical-optical double-resonance spectroscopy on a closed Λ-type three-level system to overcome Doppler broadening. A residual, broadened fluorescence background caused by velocity-changing processes in the ion beam is identified, and a background subtraction scheme implemented. At the present stage the experimental sensitivity, although already comparable with previous measurements on slower ion beams at the TSR storage ring that led to [Formula: see text] < 8.4 × 10–8, suffer from a poor signal-to-noise ratio. Modifications of the ion source as well as the detection system are discussed that promise to improve the sensitivity by one order of magnitude.
The astrophysically important molecular ions DCND and D3O + can dissociate upon capture of a free electron, a process known as dissociative recombination (DR). We give here a brief summary of recent experimental studies of the DR of these molecules that have been carried out at the TSR heavy ion storage ring.
Laser spectroscopy on high quality ion beams allows to explore physical properties of atoms and molecules and to test fundamental theories. An experiment to measure time dilation shows the potential.
We report on an energy-sensitive imaging detector for studying the fragmentation of polyatomic molecules in the dissociative recombination of fast molecular ions with electrons. The system is based on a large area (10 cm x 10 cm) position-sensitive, double-sided Si-strip detector with 128 horizontal and 128 vertical strips, whose pulse height information is read out individually. The setup allows to uniquely identify fragment masses and is thus capable of measuring branching ratios between different fragmentation channels, kinetic energy releases, as well as breakup geometries, as a function of the relative ion-electron energy. The properties of the detection system, which has been installed at the TSR storage ring facility of the Max-Planck Institute for Nuclear Physics in Heidelberg, is illustrated by an investigation of the dissociative recombination of the deuterated triatomic hydrogen cation D2H+. A huge isotope effect is observed when comparing the relative branching ratio between the D2+H and the HD+D channel; the ratio 2B(D2+H)/B(HD+D), which is measured to be 1.27 +/- 0.05 at relative electron-ion energies around 0 eV, is found to increase to 3.7 +/- 0.5 at ~5 eV.
We report the status of an experimental test of time dilation in Special Relativity. This is accomplished by simultaneously measuring the forward and backward Doppler shifts of an electronic transition of fast moving ions, using high-precision laser spectroscopy. From these two Doppler shifts both the ion velocity β = v/c and the time dilation factor can be derived. From measurements based on saturation spectroscopy on lithium ions stored at β = 0.03 and β = 0.06 in the TSR heavy-ion storage ring, we achieved an upper limit for a 𝒪[β2] deviation from Special Relativity of . In recent measurements on a β = 0.34 Li+ beam in the ESR storage ring we used optical-optical double-resonance spectroscopy which, in combination with the TSR result, gives improved sensitivity on the 𝒪[β4] term of . We discuss current limitations and possible improvements that promise an enhancement of the sensitivity by at least one order of magnitude in the future.
B. Botermann, T. Kuhl, W. Nortershauser, T. Stohlker, C. Geppert, G. Huber, S. Karpuk, C. Novotny, D. Bing, D. Schwalm, A. Wolf, G. Gwinner, T. W. Hansch, S. Reinhardt, and G. Saathoff GSI Helmholtzzentrum fur Schwerionenforschung, D-64291 Darmstadt, Germany; Institut fur Kernchemie, Johannes Gutenberg-Universitat, D-55128 Mainz, Germany; Institut fur Physik, Johannes Gutenberg-Universitat, D-55128 Mainz, Germany; Max-Planck-Institut fur Kernphysik, Saupfercheckweg 1, D-69117 Heidelberg, Germany; University of Manitoba,Winnipeg, Canada; Max-Planck-Institut fur Quantenoptik, Hans-Kopfermann-Str. 1, D-85748 Garching, Germany
Submitted for the DAMOP10 Meeting of The American Physical Society Nuclear Spin Effects in the Reactions of H3 with H2 and Electrons HOLGER KRECKEL, KYLE CRABTREE, CARRIE KAUFFMAN, BRIAN TOM, University of Illinois, OLDRICH NOVOTNY, MAX BERG, DENNIS BING, HENRIK BUHR, CLAUDE KRANTZ, MICHAEL LESTINSKY, MARIO MENDES, CHRISTIAN NORDHORN, JULIA STUTZEL, ANDREAS WOLF, MPI-K Heidelberg, RICHARD THOMAS, University of Stockholm, BENJAMIN MCCALL, University of Illinois — H3 is the simplest polyatomic molecule. It is widely used as a benchmark for theoretical calculations of molecular spectroscopy and reaction dynamics, and also plays a pivotal role as the cornerstone of interstellar chemistry. In Urbana, we have investigated the proton hop/exchange reaction H3 + H2 → (H + 5 ) ∗ → H2 + H3 for the first time at low temperatures. This reaction is the simplest bimolecular reaction involving a polyatomic, and is also the most common bimolecular reaction in the universe. Our experiments have revealed the branching ratio between proton hop and exchange, and appear to explain the observed ortho:para ratio of H3 in diffuse interstellar clouds. At the TSR storage ring of the Max Planck Institute for Nuclear Physics in Heidelberg, we have performed high-resolution measurements of the dissociative recombination (DR) cross sections of cold H3 in different mixtures of its lowest ortho and para quantum states. These measurements represent an important step towards the first state-selected DR measurements. Benjamin McCall University of Illinois at Urbana-Champaign Date submitted: 22 Jan 2010 Electronic form version 1.4
Individual product channels in the dissociative recombination of deuterated hydronium ions and cold electrons are studied in an ion storage ring by velocity imaging using spatial and mass-sensitive detection of the neutral reaction fragments. Initial and final molecular excitation are analyzed, finding the outgoing water molecules to carry internal excitation of more than 3 eV in 90% of the recombination events. Initial rotation is found to be substantial and in three-body breakup strongly asymmetric energy repartition among the deuterium products is enhanced for hot parent ions.
Ultraviolet and visible photodissociation of a vibrationally excited H(3)(+) ion beam, as produced by standard ion sources, was successfully implemented in an ion storage ring with the aim of investigating the decay of the excited molecular levels. A collinear beams configuration was used to measure the photodissociation of H(3)(+) into H(2)(+) + H fragments by transitions into the first excited singlet state with 266 and 532 nm laser beams. A clear signal could be observed up to 5 ms of storage, indicating that enough highly excited rovibrational states survive on the millisecond time scale of the experiment. The decay into H(2)(+) + H shows an effective time constant between about 1 and 1.5 ms. The initial photodissociating states are estimated to lie roughly 1 eV below the dissociation limit of 4.4 eV. The expected low population of these levels gives rise to an effective cross section of several 10(-20) cm(2) for ultraviolet and some 10(-21) cm(2) for visible light. For using multistep resonant dissociation schemes to monitor rotational populations of cold H(3)(+) in low-density environments, these measurements open promising perspectives.
We report on first measurements towards an Ives–Stilwell test of time dilation at velocities around 0.3c. In Ives–Stilwell type experiments, fast atomic ions containing a well-known transition are used as moving clocks, and time dilation as well as the velocity can be derived from the simultaneous laser-spectroscopic measurements of the Doppler shifts with and against the direction of motion. To accurately measure these Doppler shifts, the Doppler broadening caused by the ions velocity distribution needs to be overcome. We performed first feasibility studies for laser spectroscopy on 7Li+ ions in the 2s3S21 metastable ground state at the Gesellschaft für Schwerinonenforschung (GSI) in Darmstadt. The ions were stored in the Experimental Storage Ring (ESR) at a velocity of 0.338c, and optical–optical double-resonance spectroscopy on a closed Λ-type three level system was performed with two lasers propagating antiparallel to the ions motion. We found that Doppler shift measurements on a narrow subclass of the ions velocity distribution with sufficient signal-to-noise ratio are possible if the ion beam is electron-cooled and bunched. Together with the control of systematic error sources developed in our previous experiments on slower beams, the ESR experiment promises an improvement of previously achieved sensitivities to time dilation by about an order of magnitude.