0000000000352525
AUTHOR
St. Becker
Fragmentation of gold clusters stored in a penning trap
The collision-induced dissociation of positively charged gold clusters (2 to 23 atoms) stored in a Penning trap has been studied. After collisions with rare gases, excited clusters predominantly decay by emission of one or two atoms. The loss of two atoms occurs most likely through the emission of a dimer rather than a sequential evaporation. The minimum kinetic energies of clusters required to induce dissociation exhibit a pronounced odd-even effect. Clusters with an even number of delocalized electrons are more stable than the odd ones.
Photo fragmentation of metal clusters stored in a penning trap
Photo fragmentation studies of stored mass selected metal cluster ions of a large size range are reported. The experimental method and the data evaluation are described in detail. Gold cluster ions were produced by laser vaporization and stored in a Penning trap. After size selection they were electronically excited by irradiation with a pulsed laser beam. Relaxation by evaporation of neutral atoms and dimers was observed as a function of photon energy. From these data upper and lower limits for dissociation energies are determined for Aun + (n=3 to 23).
DELAYED ELECTRON EMISSION OF NEGATIVELY CHARGED TUNGSTEN CLUSTERS
The delayed electron emission of negatively charged tungsten clusters has been investigated on a time scale from 1 to 500 ms. After being stored in a Penning trap clusters ions [Formula: see text] were heated via multiphoton absorption (hν=1.81 eV). In contrast to alkali and coinage metals no photofragmentation could be detected. Instead, for all cluster sizes studied so far only a decrease in the initial ion intensity as a function of time after excitation was observed. This decrease is not caused by ion loss from the trap, but has to be attributed to neutralization via delayed electron emission. The presented results strongly suggest that this process can be viewed as “thermionic emissio…
Mass measurements of very high accuracy by time-of-flight ion cyclotron resonance of ions injected into a penning trap
Abstract The possibility of absolute mass measurements using time-of-flight detection of ion cyclotron resonance on ions injected into a Penning trap has been demonstrated. Resolving powers of 2 million have been achieved, with accuracies of about 0.5 ppm. Absolute accuracy is obtained by direct observation of the sum frequency of the cyclotron and the magnetron motions through the use of an azimuthal quadrupole r.f. field to transform initial magnetron motion into cyclotron motion. Imperfections of the Penning trap leading to systematic errors are discussed. The system has been designed specifically to measure the masses of radionuclides produced at the on-line isotope separator ISOLDE. Wi…
Fourier transform-ion cyclotron resonance mass spectrometry — A new tool for measuring highly charged ions in an electron beam ion trap
Abstract Fourier transform-ion cyclotron mass spectrometry has been applied to the study of highly charged ions produced and confined in an electron beam ion trap. Measurements of the relative ion abundance of hydrogenlike and bare krypton ions were made and compared to the abundance ratios determined with standard X-ray techniques. Good agreement was found establishing the reliability of the method as a new tool in highly charged ion research.
Resonance lonization mass spectroscopy with a pulsed thermal atomic beam
Resonance ionization mass spectroscopy (RIMS) and pulsed-laser induced desorption (PLID) have been combined for ultrasensitive detection and spectroscopy of very small samples of refractive elements. The method has been tested and applied to laser spectroscopy of 5×109 atoms (1.5 pg) of195Au (T1/2= 183d) implanted at the ISOLDE online mass separator with 60 keV into graphite. A pulsed thermal atomic beam was formed by laser desorption with a 10 ns Nd∶Yag laser pulse. Subsequently the atoms were photoionized in a three-colour, three-step resonant excitation to an autoionizing state. The selectivity was enhanced by a time-of-flight measurement of the photo ions. In resonance, one ion was dete…
Trapped metal cluster ions
An overview is given of experiments with stored metal cluster ions in a Penning trap system. The setup allows axial injection of clusters produced in an external source and a time-of-flight mass analysis of the reaction products after axial ejection. The system's options include the selection of stored ions, the manipulation of their orbits, addition of reactant and buffer gases and axial optical access for laser spectroscopic studies. As described by various examples, investigations have been made with respect to the development of trapping techniques and the characterization of metal clusters in terms of their physical and chemical properties.
Application unit for the administration of contrast gases for pulmonary magnetic resonance imaging: optimization of ventilation distribution for3He-MRI
Purpose MRI of lung airspaces using gases with MR-active nuclei (3He, 129Xe, and 19F) is an important area of research in pulmonary imaging. The volume-controlled administration of gas mixtures is important for obtaining quantitative information from MR images. State-of-the-art gas administration using plastic bags (PBs) does not allow for a precise determination of both the volume and timing of a 3He bolus. Methods A novel application unit (AU) was built according to the requirements of the German medical devices law. Integrated spirometers enable the monitoring of the inhaled gas flow. The device is particularly suited for hyperpolarized (HP) gases (e.g., storage and administration with m…
FTICR analysis of the magnetic trapping mode of the electron beam ion trap
Abstract An electron beam ion trap is used to produce and confine highly-charged atomic ions in an energetic electron beam (electron trapping mode). After switching off the electron beam the ions remain trapped due to the external magnetic and electric fields. We have investigated the properties of this magnetic trapping mode by use of Fourier transform ion cyclotron resonance mass spectrometry. We found that the number of highly charged ions and the relative species abundance is nearly the same just before and just after turning off the electron beam. The electron trapping mode thus represents an ideal method for filling the trap in situ without the losses associated with transferring the …
Fragmentation pattern of gold clusters collided with xenon atoms
Abstract The dissociation channels of gold cluster ions Au n + (2 ≤ n ≤ 23) have been investigated via collision induced dissociation in a Penning trap. Excited odd cluster ions with n ≤ 15 decay by evaporation of dimers, all others decay by monomer evaporation. Information on the binding energies is deduced from these dissociation channels.
External-ion accumulation in a Penning trap with quadrupole excitation assisted buffer gas cooling
Abstract A pulsed ion beam from an external source is injected into a Penning trap and accumulated by repeatedly lowering during ion capture to prevent the ions already captured from escaping. For the same reason the newly captured ions have to be cooled, which achieved by buffer gas collisions. To prevent radial on loss, the ions are exposed to azimuthal quadrupole excitation. By choosing the appropriate frequency (range) this method (selective quadrupole excitation assisted capture and centering (SQUEACE) allows a mass selection during the capture process and leads to a centering of those ions in the Penning trap. The multiple ion bunch capture results in a significant improvement in sign…
Cluster isobars for high-precision mass spectrometry
Doublet mass measurements of the isobars28Si3 and12C7 are performed by use of a Penning trap mass spectrometer and the Fourier transform ion cyclotron resonance (FT-ICR). The carbon and silicon cluster ions are produced by laser ablation. Results of these preliminary measurements are presented.
Collision induced dissociation of stored gold cluster ions
The stability of gold cluster ions Au + (2≦n≦23) has been investigated via collision induced dissociation in a Penning trap. Threshold energies and dissociation channels have been determined. The cluster stability exhibits a pronounced odd — even alternation: Clusters with an odd number of atoms,n, are more stable than the even-numbered ones. Enhanced stabilities are found for Au 3 + , Au 9 + , and Au 19 + in accordance with the Clemenger-Nilsson and the deformed jellium model of delocalized valence electrons. Excited odd cluster ions withn≦15 predominantly decay by evaporation of dimers; all others decay by monomer evaporation. From the dissociation channels estimates of the binding energi…
Observation of strongly deformed ground-state configurations in $^{184}$Au and $^{183}$Au by laser spectroscopy
Resonance ionization mass spectroscopy (RIMS) and pulsed-laser induced desorption (PLID) have been combined in order to study the isotope shift (IS) and hyperfine structure (HFS) of184Au (T1/2=53 s) and183Au (T1/2=42 s) in the 6s2S1/2 → 6p2P1/2 (λ=267 nm) transition. The Au isotopes were obtained as daughters in the decay of184,183Hg produced and mass separated at the new ISOLDE-3 facility at CERN. It was found that the strong deformationβ2}-0.25 setting in at186Au persists down to183Au.
Au n+-induced decomposition of N2O
Reactions between small gold cluster ions, Au, and N2O were studied in a Penning trap mass spectrometer. Gold clusters were produced by laser vaporization and injected into a Penning trap. After reaction times of 50–7000ms the products were detected by time-of-flight mass spectrometry. For the major reaction channel, Au + N2OAu1,2N + NO+, rates of (0.9±0.1)×10−12 cm3 s−1 and (2.4±0.4)×10−12 cm3 s−1 were determined which are about a factor 500 below the collision rate. The corresponding activation energies for N2O decomposition were estimated to lie below 0.6 eV and 0.3 eV. Additional products with small branching ratios were detected, viz. the ions Au1O+, Au1N2O+, Au2N+, Au2NO+, Au2N2O+, Au…