Experimental dissociation energies of metal cluster dications and their interpretation in a liquid-drop model with empirical corrections

The dissociation energies of doubly charged silver cluster ions in the size range $9l~nl~25$ are measured by multiple collision induced dissociation. They are compared to the dissociation energies of singly charged clusters. To this end, the latter are used to calculate shell corrections in a macroscopic-microscopic model. Good agreement between the resulting predictions of the dissociation energies of the doubly charged systems and the experimental values is found, which indicates the strong influence of electronic effects on the stability of small silver clusters.

Time resolved photofragmentation of Au $_{n}^{+}$ and Ag $_{n}^{+}$ clusters (n = 9, 21)

Gold and silver cluster ions were produced by laser vaporization and stored in a Penning trap. After mass selection the cluster sizes of interest were illuminated by a laser pulse and electronically excited. Photoabsorption cross sections and fragmentation patterns were measured for photon energies of 2.3 eV to 5.2 eV. Unimolecular dissociation was observed time resolved on a microsecond to millisecond scale. Dissociation energies were deduced from the measured life times.

Chemisorption of hydrogen on charged vanadium clusters

Abstract The chemisorption of hydrogen on positively charged vanadium clusters, V n + ( n = 1–17), was studied by measuring reaction rates and saturation coverages. Vanadium clusters are produced by laser vaporization and are injected into a Penning trap. Rates of the reaction V n + +H 2 → V n + H 2 are measured by axial ejection of all ions out of the trap after variable storage times and subsequent time-of-flight detection. An odd-even effect of the reaction rate is observed with odd clusters being more reactive. Clusters with low reactivity are found to be highly stable, as reflected by the respective separation energies of atoms. The number of adsorbed hydrogen atoms, m , is determined …

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.

The dissociation channels of silver clusters Agn+, 3 ≤ n ≤ 20

Abstract The low energy dissociation channels of silver cluster ions Agn+, 3 ≤ n ≤ 20 are determined by collision-induced dissociation (CID) in a Penning trap. While for most cluster sizes the first fragment cluster ion is produced by monomer evaporation, the fragment ion of small odd-sized clusters has two atoms less than their precursors indicating an evaporation of dimers. The results are compared to similar CID studies on gold cluster ions, photofragmentation patterns, abundance spectra for various silver-cluster production techniques and calculated binding energies.

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).

The trapping condition and a new instability of the ion motion in the ion cyclotron resonance trap

Abstract In analogy to the critical mass, m crit , a critical voltage, U crit , (and a general trapping parameter, π trap ) is defined, above which the ion motion in an ion cyclotron resonance (ICR) trap is unstable and the ions are lost from the trap. The theoretical values for the critical voltage are confirmed by experimental results. Singly charged gold cluster ions, Au n − , of several sizes, n = 50, 60, 76, 100, 110, and 145 (the latter corresponding to an ion mass of 28 560 u), were injected into an ICR trap, stored, and detected by axial ejection and single ion counting using a microchannel plate detector. During the storage period the trapping voltage, U , was varied for extended d…

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…

Observation of electronic and geometric shell structures of small silver clusters

Singly charged silver clusters Open image in new window in the size range n = 17 to n = 78 have been captured and stored in a Penning trap, size selected and subjected to an electron beam which leads to further ionization as well as dissociation. The resulting abundance spectra of doubly and triply charged clusters show several features: (1) A critical size for the production of doubly charged clusters which can be understood in terms of the decay pathways as previously investigated by collision induced dissociation, (2) an odd-even alternation in the abundance of singly and doubly charged clusters which inverses sign with change of charge state, (3) prominent signals for particular doubly …

ChemInform Abstract: Au+ n-Induced Decomposition of N2O.

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.

Search forBs0→μ+μ−andB0→μ+μ−Decays with CDF II

A search has been performed for B{sub s}{sup 0} {yields} {mu}{sup +}{mu}{sup -} and B{sup 0} {yields} {mu}{sup +}{mu}{sup -} decays using 7 fb{sup -1} of integrated luminosity collected by the CDF II detector at the Fermilab Tevatron collider. The observed number of B{sup 0} candidates is consistent with background-only expectations and yields an upper limit on the branching fraction of {Beta}(B{sup 0} {yields} {mu}{sup +}{mu}{sup -}) < 6.0 x 10{sup -9} at 95% confidence level. We observe an excess of B{sub s}{sup 0} candidates. The probability that the background processes alone could produce such an excess or larger is 0.27%. The probability that the combination of background and the expe…

Measurement of thett¯production cross section inpp¯collisions ats=1.96  TeVusing soft electronb-tagging

The authors present a measurement of the t{bar t} production cross section using events with one charged lepton and jets from p{bar p} collisions at a center-of-mass energy of 1.96 TeV. A b-tagging algorithm based on the probability of displaced tracks coming from the event interaction vertex is applied to identify b quarks from top decay. Using 318 pb{sup -1} of data collected with the CDF II detector, they measure the t{bar t} production cross section in events with at least one restrictive (tight) b-tagged jet and obtain 8.9{sub -1.0}{sup +1.0}(stat.){sub -1.0}{sup +1.1}(syst.) pb. The cross section value assumes a top quark mass of m{sub t} is presented in the paper. This result is cons…

Collision induced dissociation of doubly charged stored metal cluster ions

Fission barriers of doubly charged silver clusters

The monomer evaporation energies and fission barriers of doubly charged silver cluster ions in the size range 9≤n≤25 are measured by collision induced dissociation. They are compared to the dissociation energies of singly charged silver clusters. A macroscopic liquid drop model combined with empirical microscopic corrections successfully describes the measured fission barriers.

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.

Production and investigation of multiply charged metal clusters in a Penning trap

Singly charged gold cluster ions from a laser-vaporization source are transferred into a Penning trap and subjected to electron bombardment. The charged reaction products are analyzed by time-of-flight mass spectrometry after axial ejection from the trap. They include singly charged cluster fragments, multiply charged clusters of the initial size and multiply charged cluster fragments. The multiply charged clusters are selected and further investigated by collision induced dissociation. Two types of reactions can be distinguished: Dissociation into several charged fragments and evaporation of neutrals. Several features of multiply charged clusters relevant for future investigations are revi…

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…

Chemisorption of hydrogen on a V5+ cluster

Abstract The binding between V 5 + and hydrogen is studied by collision induced dissociation of the cluster-adsorbate V 5 + H 2 . Vanadium clusters are produced by laser vaporization and injected into an electromagnetic ion trap. After mass separation of V 5 + , the pulsed addition of hydrogen yields V 5 + H 2 . The desorption of hydrogen is studied by acceleration of V 5 + H 2 with variable rf voltages and collisions with argon atoms. From the threshold voltage necessary for dissociation a binding energy of H 2 on V 5 + of 2.4 ± 0.3 eV is estimated. This value is consistent with a dissociative chemisorption of hydrogen.

Low-energy decay pathways of doubly charged silver clusters $Ag_{n}^{2+}$ (n = 9 - 24)

The low-energy dissociation channels of mass selected silver cluster ions Ag n 2+ (n = 9–24) are determined by collision induced dissociation (CID) in a Penning trap. While all clusters of the size n ≥ 17 evaporate neutral monomers, most smaller clusters undergo asymmetric fission of the form Ag n 2+ → Ag −3 + + Ag {3} + . However, Ag 15 2+ and Ag 11 2+ emit monomers which indicates shell or odd-even effects. The observed fragmentation pathways are different from previous reports of measurements with sputtered Ag n 2+ .

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…

Decay pathway determination of even-size dicationic silver clusters: Ag162+ and Ag182+ revisited by pre-precursor selection and sequential decay

Abstract It is demonstrated how by selection of pre-precursor cluster ions Ag 2 n +1 2+ and collision-induced dissociation an ensemble of Ag 2 n 2+ can be produced, which is not contaminated by Ag n + clusters of the same size-to-charge state ratio, n / z . By use of this technique, Ag 16 2+ and Ag 18 2+ precursor ensembles have been prepared for further investigations. They are observed to decay by neutral monomer evaporation, Ag 2 n 2+ →Ag 2 n −1 2+ +Ag, and trimer fission, Ag 2 n 2+ →Ag 2 n −3 + +Ag 3 + , and show no sign of symmetric fission.

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…