Towards high-accuracy mass spectrometry of highly charged short-lived ions at ISOLTRAP

Dedicated to H.-J. Kluge on the occasion of his 65th birthday anniversary - Jürgen Kluge Special Issue; Multiply charged ions of stable xenon isotopes from a plasma ion source have been mass-selected by the on-line mass separator ISOLDE/CERN and delivered to the triple-trap mass spectrometer ISOLTRAP. The doubly charged ions that survived the charge-exchange processes during bunching and ion preparation were transferred to a precision Penning trap for mass determination. Mass values were obtained for the isotopes with mass numbers A=126,129,130,136. They are consistent with previous results except for the case of $^{126}Xe$ where a significant deviation from the literature value was found. …

High-accuracy mass determination of unstable cesium and barium isotopes

Direct mass measurements of short-lived Cs and Ba isotopes have been performed with the tandem Penning trap mass spectrometer ISOLTRAP installed at the on-line isotope separator ISOLDE at CERN. Typically, a mass resolving power of 600 000 and an accuracy of $\delta \mbox{m} \approx 13$ keV have been obtained. The masses of $^{123,124,126}$Ba and $^{122m}$Cs were measured for the first time. A least-squares adjustment has been performed and the experimental masses are compared with theoretical ones, particularly in the frame of a macroscopic-microscopic model.

Pulsed photodissociation in an ion cyclotron resonance trap: extending the time range for unimolecular dissociation studies of metal clusters

The Ramsey method in high-precision mass spectrometry with Penning traps: Experimental results

The highest precision in direct mass measurements is obtained with Penning trap mass spectrometry. Most experiments use the interconversion of the magnetron and cyclotron motional modes of the stored ion due to excitation by external radiofrequency-quadrupole fields. In this work a new excitation scheme, Ramsey's method of time-separated oscillatory fields, has been successfully tested. It has been shown to reduce significantly the uncertainty in the determination of the cyclotron frequency and thus of the ion mass of interest. The theoretical description of the ion motion excited with Ramsey's method in a Penning trap and subsequently the calculation of the resonance line shapes for differ…

First Observation of Multiply Charged Vanadium Clusters in a Penning Trap

Laser Investigations of Stored Metal Cluster Ions

The combination of ion storage in a Penning trap and photoexcitation by pulsed lasers has proven to be a versatile instrument in metal cluster research. Recent experiments which make use of both components allow a detailed study of the clusters' properties. In particular, a new method to measure dissociation energies is reviewed and preliminary results on the competition between electron emission and neutral monomer evaporation from dianionic metal clusters are presented.

On-line commissioning of SHIPTRAP

Abstract The on-line commissioning of the Penning-trap mass spectrometer SHIPTRAP was successfully completed with a mass measurement of holmium and erbium radionuclides produced at SHIP. A large fraction of contaminant ions created in the stopping cell was identified to originate from the buffer-gas supply system. Using a liquid nitrogen cold trap they were reduced to a tolerable amount and mass measurements of Er 147 , Er 148 , and Ho 147 with relative uncertainties of about 1 × 1 0 − 6 were performed.

EBIT trapping program

The LLNL electron beam ion trap provides the world's only source of stationary highly charged ions up to bare U. This unique capability makes many new atomic and nuclear physics experiments possible.

Electron impact ionization/dissociation of size selected gold cluster cations

Abstract Singly charged gold clusters, Au n + in the size range n =12 to 72 have been captured and stored in a Penning trap, size selected and subjected to an electron beam. This interaction leads to further ionization as well as dissociation. The resulting abundance spectra of doubly and triply charged clusters show (a) a lower size limit for the production of multiply charged clusters from an ensemble of hot precursors, which can be understood in terms of the respective decay pathways, (b) an odd/even alternation of singly and doubly charged clusters in the size range below n =30, which inverses sign with change of charge state, and (c) magic numbers, i.e. prominent signals for particular…

Laser Spectroscopy of Neutron-Rich Hg207,208 Isotopes: Illuminating the Kink and Odd-Even Staggering in Charge Radii across the N=126 Shell Closure

The mean-square charge radii of $^{207,208}$Hg ($Z=80, N=127,128$) have been studied for the first time and those of $^{202,203,206}$Hg ($N=122,123,126$) remeasured by the application of in-source resonance-ionization laser spectroscopy at ISOLDE (CERN). The characteristic \textit{kink} in the charge radii at the $N=126$ neutron shell closure has been revealed, providing the first information on its behavior below the $Z=82$ proton shell closure. A theoretical analysis has been performed within relativistic Hartree-Bogoliubov and non-relativistic Hartree-Fock-Bogoliubov approaches, considering both the new mercury results and existing lead data. Contrary to previous interpretations, it is d…

Trianionic gold clusters

Using Penning-trap experiments and a shell-correction method incorporating ellipsoidal shape deformations, we investigate the formation and stability patterns of trianionic gold clusters. Theory and ex- periment are in remarkable agreement concerning appearance sizes and electronic shell eects. In contrast to multiply cationic clusters, decay of the trianionic gold clusters occurs primarily via electron autodetach- ment and tunneling through a Coulomb barrier, rather than via ssion. PACS. 36.40.Wa Charged clusters { 36.40.Qv Stability and fragmentation of clusters { 36.40.Cg Electronic and magnetic properties of clusters

Mass spectrometry and decay spectroscopy of isomers across the Z=82 shell closure

Recent results from a measurement campaign studying the isomerism in neutron-deficient Tl isotopes are presented. The measurements make use of a nuclear spectroscopy setup coupled to the high-resolution Penning-trap mass spectrometer ISOLTRAP at CERN's radioactive ion-beam facility ISOLDE. The mass values of 190,194Tl are improved and a mass-spin-state assignment is carried out. An additional mass measurement of the grandparent nuclide 198At allows the deduction of the spin-state ordering in 190Tl. As a result, the excitation energies of the isomers in both Tl isotopes are determined for the first time to Eex(194Tl)=260(15) keV and E ex(190Tl)=89(12) keV. Furthermore, this allows anchoring …

ISOLTRAP mass measurements of exotic nuclides at

The ISOLTRAP experiment at the ISOLDE facility at CERN is a Penning trap mass spectrometer for on-line mass measurements on short-lived radionuclides. It allows the determination of atomic masses of exotic nuclides with a relative uncertainty of only 10−8. The results provide important information for, e.g., weak interaction studies and nuclear models. Recent ISOLTRAP investigations and applications of high-precision mass measurements are discussed.

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.

The NEXT Project: Towards Production and Investigation of Neutron-Rich Heavy Nuclides

The heaviest actinide elements are only accessible in accelerator-based experiments on a one-atom-at-a-time level. Usually, fusion–evaporation reactions are applied to reach these elements. However, access to the neutron-rich isotopes is limited. An alternative reaction mechanism to fusion–evaporation is multinucleon transfer, which features higher cross-sections. The main drawback of this technique is the wide angular distribution of the transfer products, which makes it challenging to catch and prepare them for precision measurements. To overcome this obstacle, we are building the NEXT experiment: a solenoid magnet is used to separate the different transfer products and to focus those of …

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 …

Decay pathways of small gold clusters

The decay pathway competition between monomer and dimer evaporation of photoexcited cluster ions Au + n, n = 2-27, has been investigated by photodissociation of size-selected gold clusters stored in a Penning trap. For n > 6 the two decay pathways are distinguished by their experimental signature in time-resolved measurements of the dissociation. For the smaller clusters, simple fragment spectra were used. As in the case of the other copper-group elements, even-numbered gold cluster ions decay exclusively by monomer evaporation, irrespective of their size. For small odd-size gold clusters, dimer evaporation is a competitive alternative, and the smaller the odd-sized clusters, the more likel…

Recent developments for high-precision mass measurements of the heaviest elements at SHIPTRAP

Abstract Atomic nuclei far from stability continue to challenge our understanding. For example, theoretical models have predicted an “island of stability” in the region of the superheavy elements due to the closure of spherical proton and neutron shells. Depending on the model, these are expected at Z = 114, 120 or even 126 and N = 172 or 184. Valuable information on the road to the island of stability is derived from high-precision mass measurements, which give direct access to binding energies of short-lived trans-uranium nuclei. Recently, direct mass measurements at SHIPTRAP have been extended to nobelium and lawrencium isotopes around the deformed shell gap N = 152. In order to further …

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.

Pulsed gas injection for X-ray spectroscopy of highly charged ions stored in the magnetic trapping mode of an electron beam ion trap

Abstract Highly charged atoms produced in an electron beam ion trap were stored after the electron beam was turned off by operating the trap in the magnetic trapping mode. Such storage allowed monitoring charge exchange reactions between the stored ions and residual neutral gas present in the trap by X-ray detection. The charge exchange reactions were enhanced by the application of a pulse of neutral gas. The method was exemplified for the case of H-like uranium interacting with neutral neon, where the K-shell X-rays and the series limit for the electron capture of U91+ were observed.

Quantum-state-selective decay spectroscopy of Ra213

An experimental scheme combining the mass resolving power of a Penning trap with contemporary decay spectroscopy has been established at GSI Darmstadt. The Universal Linear Accelerator (UNILAC) at GSI Darmstadt provided a $^{48}\mathrm{Ca}$ beam impinging on a thin $^{170}\mathrm{Er}$ target foil. Subsequent to velocity filtering of reaction products in the Separator for Heavy Ion reaction Products (SHIP), the nuclear ground state of the $5n$ evaporation channel $^{213}\mathrm{Ra}$ was mass-selected in SHIPTRAP, and the $^{213}\mathrm{Ra}$ ions were finally transferred into an array of silicon strip detectors surrounded by large composite germanium detectors. Based on comprehensive geant4 s…

Precision Mass Measurements of Cr58–63 : Nuclear Collectivity Towards the N=40 Island of Inversion

The neutron-rich isotopes $^{58-63}$Cr were produced for the first time at the ISOLDE facility and their masses were measured with the ISOLTRAP spectrometer. The new values are up to 300 times more precise than those in the literature and indicate significantly different nuclear structure from the new mass-surface trend. A gradual onset of deformation is found in this proton and neutron mid-shell region, which is a gateway to the second island of inversion around \emph{N}=40. In addition to comparisons with density-functional theory and large-scale shell-model calculations, we present predictions from the valence-space formulation of the \emph{ab initio} in-medium similarity renormalization…

Recent Exploits of the ISOLTRAP Mass Spectrometer

Abstract The Penning-trap mass spectrometer ISOLTRAP, located at the isotope-separator facility ISOLDE (CERN), is presented in its current form taking into account technical developments since 2007. Three areas of developments are presented. The reference ion sources have been modified to guarantee a sufficient supply of reference ions for mass measurements and systematic studies. Different excitation schemes have been investigated for manipulation of the ion motion in the Penning trap, to enhance either the purification or measurement process. A multi-reflection time-of-flight mass separator has been implemented and can now be routinely used for purification and as a versatile tool for bea…

New developments of the in-source spectroscopy method at RILIS/ISOLDE

At the CERN ISOLDE facility, long isotope chains of many elements are produced by proton-induced reactions in target materials such as uranium carbide. The Resonance Ionization Laser Ion Source (RILIS) is an efficient and selective means of ionizing the reaction products to produce an ion beam of a chosen isotope. Coupling the RILIS with modern ion detection techniques enables highly sensitive studies of nuclear properties (spins, electromagnetic moments and charge radii) along an isotope chain, provided that the isotope shifts and hyperfine structure splitting of the atomic transitions can be resolved. At ISOLDE the campaign to measure the systematics of isotopes in the lead region (Pb, Bi…

Model-free determination of dissociation energies of polyatomic systems.

We describe and apply a new procedure that allows a direct determination of dissociation energies of polyatomic systems (clusters, fullerenes, polymers, and other molecules) without any modeling of the systems under investigation. As an example, we have determined the dissociation energies of a series of gold clusters Au(+)n. A comparison with values obtained from statistical models of unimolecular dissociation shows that these models significantly fail to describe the data. In contrast, the new method yields values which are an order of magnitude more accurate, thus allowing one to experimentally set benchmarks for any theory which attempts to describe activated processes.

Internal ion impact ionization for Fourier-transform ion cyclotron resonance

A general scheme for ionization and fragmentation of ions in Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICRMS) is introduced. The technique is based upon excitation of high-frequency (i.e. lowmass) primary ions (e.g. N, Al+, H2O+·) which may be generated by standard ionization methods (e.g. electron ionization or laser desorption) inside the trap. Generation of the primary ions is followed by excitation of their cyclotron motion to high translational energy to serve as projectile ions. The projectiles serve two functions: to ionize neutral gas atoms and/or molecules (secondary ions) within the trap internal ion impact ionization (IIII), and to collisionally activate the…

The temperature dependence of photoabsorption of V13+

Photoabsorption cross sections of trapped V 13 + clusters were measured for energies between 1.4 eV and 6.1 eV by use of a two-photon fragmentation technique. Using two laser pulses separated by a 100-ns delay period the cross sections of hot clusters (up to 1800 K) could be compared to the values at room temperature. Whereas sodium clusters are known to exhibit pronounced temperature dependence below 300 K, no continuation of these effects to higher temperatures was found for V 13 + .

A Penning Trap for Studying Cluster Ions

We propose to use a Penning trap for spectroscopy of stored cluster ions. A similar device has been built for the purpose of mass measurements of short-lived nuclei produced at the on-line isotope separator ISOLDE/CERN. A resolving power of 500,000 in a mass measurement of39K and an accuracy of 2 × 10−7 for the85Rb/39K mass ratio were obtained. An efficiency for in-flight capture as high as 70% was achieved. The method provides very high sensitivity since typically only 10 to 100 ions are stored in the trap. We intend to perform laser spectroscopy on trapped Na clusters as a first application of the trap technique.

The cryogenic gas stopping cell of SHIPTRAP

The overall efficiency of the Penning-trap mass spectrometer SHIPTRAP at GSI Darmstadt, employed for high-precision mass measurements of exotic nuclei in the mass region above fermium, is presently mostly limited by the stopping and extraction of fusion-evaporation products in the SHIPTRAP gas cell. To overcome this limitation a second-generation gas cell with increased stopping volume was designed. In addition, its operation at cryogenic temperatures leads to a higher gas density at a given pressure and an improved cleanliness of the helium buffer gas. Here, the results of experiments with a 219Rn recoil ion source are presented. An extraction efficiency of 74(3)% was obtained, a significa…

Towards a magnetic field stabilization at ISOLTRAP for high-accuracy mass measurements on exotic nuclides

Abstract The field stability of a mass spectrometer plays a crucial role in the accuracy of mass measurements. In the case of mass determination of short-lived nuclides with a Penning trap, major causes of fluctuations are temperature variations in the vicinity of the trap and pressure changes in the liquid helium cryostat of the superconducting magnet. Thus systems for the temperature and pressure stabilization of the Penning trap mass spectrometer ISOLTRAP at the ISOLDE facility at CERN have been installed. A reduction of the temperature and pressure fluctuations by at least an order of magnitude down to Δ T ≈ ± 5 mK and Δ p ≈ ± 5 Pa has been achieved, which corresponds to a relative magn…

Examining the N=28 shell closure through high-precision mass measurements of Ar46–48

The strength of the $N=28$ magic number in neutron-rich argon isotopes is examined through high-precision mass measurements of $^{46\text{--}48}\mathrm{Ar}$, performed with the ISOLTRAP mass spectrometer at ISOLDE/CERN. The new mass values are up to 90 times more precise than previous measurements. While they suggest the persistence of the $N=28$ shell closure for argon, we show that this conclusion has to be nuanced in light of the wealth of spectroscopic data and theoretical investigations performed with the SDPF-U phenomenological shell model interaction. Our results are also compared with ab initio calculations using the valence space in-medium similarity renormalization group and the s…

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.

Isoltrap pins down masses of exotic nuclides

The mass of radionuclides contribute to a variety of fundamental studies including tests of the weak interaction and the Standard Model. The limits of mass measurements of exotic nuclides have been extended considerably by the Penning-trap mass spectrometer ISOLTRAP at the ISOLDE facility at CERN. Recent ISOLTRAP measurements are summarized and current technical improvements are outlined.

Electronic effects in the production of smali dianionic gold clusters by electron attachment on to stored Au-n, n = 12-28

Abstract Single charged gold clusters Au n -, 12  n  28, are stored in a Penning trap, size selected and transformed into dianions, Au2- n by the application of an electron beam. At the onset of dianion production, that is that range of cluster sizes n where the smallest doubly charged clusters are observed, the measured intensity ratio of the dianions to their precursors is not a continuous function of cluster size. Instead, there is a strong odd-even effect and a comparatively intense signal of Au2-18 The observed structures are very reminiscent of similar phenomena in the abundance spectra of metal clusters as observed by Knight et al. (1984, Phys. Rev. Lett., 52, 2141), which gave ris…

Surveying the N=40 island of inversion with new manganese masses

High-precision mass measurements of neutron-rich 57−66Mn and 61−63Fe isotopes are reported. The new mass surface shows no shell closure at N=40. In contrast, there is an increase of the two-neutron separation energy at N=38. This behavior is consistent with the onset of collectivity due to the occupation of intruder states from higher orbits, in analogy with the well known “island of inversion” around N=20. Our results indicate that the neutron-rich Mn isotopes, starting from 63Mn, are most likely within the new island of inversion. From the new mass surface, we evaluate the empirical proton-neutron interaction and the pairing gap, both playing a significant role in the structural changes i…

Multisequential photofragmentation of size-selected gold cluster ions

Time-resolved fragmentation measurements have been performed on stored, size-selected gold cluster ions ${\mathrm{Au}}_{n}^{+}$ $(n=17--21)$ that have been excited up to 15 eV by multiphoton absorption. These excitation energies are far above the clusters' dissociation thresholds and initiate multistep sequential unimolecular dissociation by evaporation of neutral monomers. The measurements allow for the determination of a combination of kinetic-energy release and radiative cooling of the excited clusters. Also, previously determined model-independent values of the cluster dissociation energies are confirmed by the present measurements. The data are consistent with thermal values of the kin…

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).

Penning-trap mass spectrometry and mean-field study of nuclear shape coexistence in the neutron-deficient lead region

We present a study of nuclear shape coexistence in the region of neutron-deficient lead isotopes. The midshell gold isotopes 180,185,188,190Au (Z=79), the two long-lived nuclear states in 197At (Z=85), and the neutron-rich nuclide 219At were produced by the ISOLDE facility at CERN and their masses were determined with the high-precision Penning-trap mass spectrometer ISOLTRAP. The studied gold isotopes address the trend of binding energies in a region of the nuclear chart where the nuclear charge radii show pronounced discontinuities. Significant deviations from the atomic-mass evaluation were found for 188,190Au. The new trend of two-neutron separation energies is smoother, although it doe…

New approaches to stored cluster ions

Ion traps are “wall-less containers” which allow the extended storage of selected species. During the storage various interaction steps may be repeatedly applied. To this end no further hardware has to be added - in contrast to beam experiments. In this progress report two examples of recent developments are presented: the experiments have been performed with metal clusters stored in a Penning (ion cyclotron resonance) trap. A new experimental scheme has been developed which allows precision measurements of the dissociation energies of polyatomic species. It has been triggered by investigations on the delayed photodissociation of stored metal clusters. However, the technique is also readily…

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…

Probing the nuclide 180W for neutrinoless double-electron capture exploration

Abstract The mass difference of the nuclides 180 W and 180 Hf has been measured with the Penning-trap mass spectrometer SHIPTRAP to investigate 180 W as a possible candidate for the search for neutrinoless double-electron capture. The Q ϵ ϵ -value was measured to 143.20(27) keV. This value in combination with the calculations of the atomic electron wave functions and other parameters results in a half-life of the 0 + → 0 + ground-state to ground-state double-electron capture transition of approximately 5 × 10 27 years / 〈 m ϵ ϵ [ eV ] 〉 2 .

Double-βtransformations in isobaric triplets with mass numbersA=124, 130, and 136

The Q values of double-electron capture in ${}^{124}$Xe, ${}^{130}$Ba, and ${}^{136}$Ce and double-beta decay of ${}^{124}$Sn and ${}^{130}$Te have been determined with the Penning-trap mass spectrometer SHIPTRAP with a few hundred eV uncertainty. These nuclides are members of three isobaric triplets with common daughter nuclides. The main goal of this work was to investigate the existence of the resonant enhancement of the neutrinoless double-electron-capture rates in ${}^{124}$Xe and ${}^{130}$Ba in order to assess their suitability for the search for neutrinoless double-electron capture. Based on our results, in neither of these cases is the resonance condition fulfilled.

Multiply charged metal cluster anions

Formation, stability patterns, and decay channels of silver dianionic and gold trianionic clusters are investigated with Penning-trap experiments and a shell-correction method including shape deformations. The theoretical predictions pertaining to the appearance sizes and electronic shell effects are in remarkable agreement with the experiments. Decay of the multiply anionic clusters occurs predominantly by electron tunneling through a Coulomb barrier, rather than via fission, leading to appearance sizes unrelated to those of multiply cationic clusters.

Model-independent determination of dissociation energies: method and applications

A number of methods are available for the purpose of extracting dissociation energies of polyatomic particles. Many of these techniques relate the rate of disintegration at a known excitation energy to the value of the dissociation energy. However, such a determination is susceptible to systematic uncertainties, mainly due to the unknown thermal properties of the particles and the potential existence of 'dark' channels, such as radiative cooling. These problems can be avoided with a recently developed procedure, which applies energy-dependent reactions of the decay products as an uncalibrated thermometer. Thus, it allows a direct measurement of dissociation energies, without any assumption …

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…

Critical-Point Boundary for the Nuclear Quantum Phase Transition NearA=100from Mass Measurements ofKr96,97

Mass measurements of (96,97)Kr using the ISOLTRAP Penning-trap spectrometer at CERN-ISOLDE are reported, extending the mass surface beyond N=60 for Z=36. These new results show behavior in sharp contrast to the heavier neighbors where a sudden and intense deformation is present. We interpret this as the establishment of a nuclear quantum phase transition critical-point boundary. The new masses confirm findings from nuclear mean-square charge-radius measurements up to N=60 but are at variance with conclusions from recent gamma-ray spectroscopy.

Theory of quadrupole detection fourier transform-ion cyclotron resonance

Abstract The theoretical basis of the recently introduced quadrupole detection Fourier transform-ion cyclotron resonance technique is developed by use of the concept of image charges induced in the detection electrodes. The appearance of resonances at frequencies 2ω+, 2ω−, (ω+ + ω−) and (ω+ − ω−) is explained. The new method is compared with the standard (dipole) detection scheme. Techniques are suggested allowing the simultaneous determination of all resonance frequencies ω+ (perturbed, or reduced, cyclotron frequency), ω− (magnetron frequency) and ωz (trapping frequency).

Investigation of Space-Charge Phenomena in Gas-Filled Penning Traps

The centering of ions in Penning traps by a quadrupolar radiofrequency excitation in the presence of a buffer gas has been studied in the regime of high charge‐densities. It is found to deviate significantly from the single‐particle situation. In particular, the efficiency of the cooling process is affected as well as the resolving power. The behavior has been studied experimentally at the preparation trap REXTRAP and the high‐precision Penning trap setup ISOLTRAP both located at the on‐line mass separator ISOLDE at CERN. In addition, the phenomenon has been investigated numerically by a custom‐designed simulation.

Absolute cross-sections for the nonresonant multi-photon ionization of toluene and xylene in the gas phase

Abstract The absolute multi-photon ionization cross-section of the phenyl ring was determined by laser-ionization of toluene and xylene molecules in the gas phase. Excitation was achieved using nonresonant four-photon absorption of the frequency doubled light of a 10 ns pulsed Nd:YAG laser (532 nm). The resulting ions were stored in a Penning trap and detected by time-of-flight mass spectrometry. The values of the cross-sections are 1.4(3)×10 −42 cm 8 W −4 s −1 and 1.3(3)×10 −42 cm 8 W −4 s −1 for toluene and xylene, respectively.

First Fourier-transform ion cyclotron resonance signals of very highly charged atomic ions

We report on the first application of Fourier-transform ion cyclotron resonance mass spectrometry to the very highly charged ions produced in the high-energy electron beam ion trap (SuperEBIT) at the Lawrence Livermore National Laboratory. Initial results are described, and spectra are presented from ions as highly charged as Cs53+.

Charge radii, moments, and masses of mercury isotopes across the N=126 shell closure

Combining laser spectroscopy in a Versatile Arc Discharge and Laser Ion Source, with Penning-trap mass spectrometry at the CERN-ISOLDE facility, this work reports on mean-square charge radii of neutron-rich mercury isotopes across the $N = 126$ shell closure, the electromagnetic moments of $^{207}$Hg and more precise mass values of $^{206-208}$Hg. The odd-even staggering (OES) of the mean square charge radii and the kink at $N = 126$ are analyzed within the framework of covariant density functional theory (CDFT), with comparisons between different functionals to investigate the dependence of the results on the underlying single-particle structure. The observed features are defined predomina…

Dissociation energies of silver clusters Agn+, n=14, 15, 16, 18

A recently developed method to determine dissociation energies has been applied to positively charged silver clusters of size n=14, 15, 16 and 18. The method uses a combination of sequential and single step decays. It requires an uncalibrated thermometer which here is provided by the evaporation rate constants of the product clusters. For this purpose, earlier measurements [J. Chem. Phys. 57 (1998) 2786] are reanalyzed with the new method. The resulting dissociation energies are compared with the liquid drop values and the measured decay rate constants with expected rate constants from detailed balance theory.

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 …

Photodissociation of small group-11 metal cluster ions: Fragmentation pathways and photoabsorption cross sections

Noble metal cluster ions Cu(n)(+), Ag(n)(+) and Au(n)(+) (n = 3-21) have been stored in a Penning trap and photodissociated by low intensity laser pulses of 10 ns at photon energies of 3.49 eV and 4.66 eV. The fragmentation pathways, neutral monomer and dimer evaporation, have been monitored as a function of cluster size, excitation energy and element. It is found that the behavior of the branching ratio between monomer and dimer evaporation as a function of excitation energy depends on the metal under investigation. In particular, the slope of the energy dependence is positive for silver but negative for gold and copper cluster ions. Furthermore, photoabsorption cross sections are determin…

First Glimpse of the N=82 Shell Closure below Z=50 from Masses of Neutron-Rich Cadmium Isotopes and Isomers

We probe the $N=82$ nuclear shell closure by mass measurements of neutron-rich cadmium isotopes with the ISOLTRAP spectrometer at ISOLDE-CERN. The new mass of $^{132}\mathrm{Cd}$ offers the first value of the $N=82$, two-neutron shell gap below $Z=50$ and confirms the phenomenon of mutually enhanced magicity at $^{132}\mathrm{Sn}$. Using the recently implemented phase-imaging ion-cyclotron-resonance method, the ordering of the low-lying isomers in $^{129}\mathrm{Cd}$ and their energies are determined. The new experimental findings are used to test large-scale shell-model, mean-field, and beyond-mean-field calculations, as well as the ab initio valence-space in-medium similarity renormalizat…

Shape staggering of midshell mercury isotopes from in-source laser spectroscopy compared with density-functional-theory and Monte Carlo shell-model calculations

Neutron-deficient Hg177-185 isotopes were studied using in-source laser resonance-ionization spectroscopy at the CERN-ISOLDE radioactive ion-beam facility in an experiment combining different detection methods tailored to the studied isotopes. These include either α-decay tagging or multireflection time-of-flight gating for isotope identification. The endpoint of the odd-even nuclear shape staggering in mercury was observed directly by measuring for the first time the isotope shifts and hyperfine structures of Hg177-180. Changes in the mean-square charge radii for all mentioned isotopes, magnetic dipole, and electric quadrupole moments of the odd-A isotopes and arguments in favor of I=7/2 s…

Buffer-gas-free mass-selective ion centering in Penning traps by simultaneous dipolar excitation of magnetron motion and quadrupolar excitation for interconversion between magnetron and cyclotron motion

A new excitation scheme of the radial ion-motional modes is introduced for Penning-trap ion-cyclotron-resonance experiments. By simultaneous dipolar excitation of the magnetron motion and resonant quadrupolar excitation for the conversion between magnetron motion and cyclotron motion, a mass-selective recentering of the ions of interest is performed while all other (contaminant) ions are ejected from the trap. This new technique does not rely on the application of a buffer gas as presently used [G. Savard, St. Becker, G. Bollen, H.-J. Kluge, R.B. Moore, Th. Otto, L Schweikhard, H. Stolzenberg, U. Wiess, Physics Letters A 158 (1991) 247] and will thus prevent charge-exchange reactions and da…

Resonant enhancement of neutrinoless double-electron capture in 152Gd.

In the search for the nuclide with the largest probability for neutrinoless double-electron capture, we have determined the ${Q}_{ϵϵ}$ value between the ground states of $^{152}\mathrm{Gd}$ and $^{152}\mathrm{Sm}$ by Penning-trap mass-ratio measurements. The new ${Q}_{ϵϵ}$ value of 55.70(18) keV results in a half-life of ${10}^{26}\text{ }\text{ }\mathrm{yr}$ for a 1 eV neutrino mass. With this smallest half-life among known $0\ensuremath{\nu}ϵϵ$ transitions, $^{152}\mathrm{Gd}$ is a promising candidate for the search for neutrinoless double-electron capture.

Time-separated oscillatory fields for high-precision mass measurements on short-lived Al and Ca nuclides

High-precision Penning trap mass measurements on the stable nuclide 27Al as well as on the short-lived radionuclides 26Al and 38,39Ca have been performed by use of radiofrequency excitation with time-separated oscillatory fields, i.e. Ramsey's method, as recently introduced for the excitation of the ion motion in a Penning trap, was applied. A comparison with the conventional method of a single continuous excitation demonstrates its advantage of up to ten times shorter measurements. The new mass values of 26,27Al clarify conflicting data in this specific mass region. In addition, the resulting mass values of the superallowed beta-emitter 38Ca as well as of the groundstate of the beta-emitte…

The influence of internal degrees of freedom on the unimolecular decay of the molecule–cluster compound Au8+CH3OH

Time-resolved photodissociation measurements of the sequential reaction Au8+CH3OH→Au8+→Au7+ and the direct reaction Au8+→Au7+ have been performed for several excitation energies. The production rates and yields of the final state Au7+ in the sequential process are strongly influenced by the excitation energy deposited into the evaporated methanol molecule during the initial fragmentation step. Both the rate constants and yields can be fitted with a single parameter, the cluster–methanol binding energy.

First absolute mass measurements of short-lived isotopes

Absolute mass measurements of short-lived isotopes have been performed at the on-line mass separator ISOLDE at CERN by determining the cyclotron frequencies of ions confined in a Penning trap. The cyclotron frequencies for77,78,85,86,88Rb and88Sr ions could be determined with a resolving power of 3×105 and an accuracy of better than 10−6, which corresponds to 100 keV for massA=100. The shortest-lived isotope under investigation was77Rb with a half-life of 3.7 min. The resonances obtained for the isobars88Rb and88Sr were clearly resolved.

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

Highly-charged ions in a penning trap: mass measurements, etc.

The use of a Penning trap will start a new generation of precision experiments on highly charged ions. The long storage time of the ions in combination with a controlled confinement in a very small volume will enable accuracies in mass determination better than δm/m = 10-8.

Laser desorption/ionization cluster studies for calibration in mass spectrometry

Precise mass calibration is mandatory in many fields of mass spectrometry. We have performed laser desorption/ionization cluster studies with a MALDI-TOF mass spectrometer on gold and fullerene targets to produce atomic clusters. These investigations demonstrate that clusters are ideally suited for this purpose. Pulsed N 2 -laser and Nd:YAG-laser ablation was used to produce positively as well as negatively charged clusters. Earlier observations of dianionic metal clusters are confirmed. First results from the tandem Penning trap mass spectrometer ISOLTRAP using carbon clusters as mass references show how carbon clusters can be applied to precision mass spectrometry by providing absolute ma…

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.

Direct mass measurements above uranium bridge the gap to the island of stability

The mass of an atom incorporates all its constituents and their interactions. The difference between the mass of an atom and the sum of its building blocks (the binding energy) is a manifestation of Einstein's famous relation E = mc(2). The binding energy determines the energy available for nuclear reactions and decays (and thus the creation of elements by stellar nucleosynthesis), and holds the key to the fundamental question of how heavy the elements can be. Superheavy elements have been observed in challenging production experiments, but our present knowledge of the binding energy of these nuclides is based only on the detection of their decay products. The reconstruction from extended d…

Production and trapping of carbon clusters for absolute mass measurements at ISOLTRAP

Singly-charged carbon clusters C/sub n//sup +/ (n >or= 1) have been produced by laser-induced desorption and fragmentation of C/sub 60/ fullerenes and have been injected into and stored in the Penning trap system of the ISOLTRAP mass spectrometer at ISOLDE/CERN. The present study is the first step to extend the until now direct mass measurements at ISOLTRAP to absolute mass measurements by using clusters of /sup 12/C. (10 refs).

Approaching theN=82shell closure with mass measurements of Ag and Cd isotopes

Mass measurements of neutron-rich Cd and Ag isotopes were performed with the Penning trap mass spectrometer ISOLTRAP. The masses of ${}^{112,114\ensuremath{-}124}$Ag and ${}^{114,120,122\ensuremath{-}124,126,128}$Cd, determined with relative uncertainties between $2\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}8}$ and $2\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}7}$, resulted in significant corrections and improvements of the mass surface. In particular, the mass of $^{124}\mathrm{Ag}$ was previously unknown. In addition, other masses that had to be inferred from $Q$ values of nuclear decays and reactions have now been measured directly. The analysis includes various mass…

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.

Observation of multiply charged silver-cluster anions

Singly charged silver-cluster anions are produced in a laser vaporization source and transferred into a Penning trap. After size selection the clusters are subjected to an electron bath in the trap, which results in the attachment of further electrons. The relative abundance of dianions or trianions as a function of the clusters' size is analyzed by time-of-flight mass spectrometry. Silver-cluster dianions are observed for sizes n≥ 24 and trianions for n > 100. In addition, a detailed study of the cluster sizes 24 ?n? 60 shows a pronounced resistance to electron attachment for singly charged anions Agn- with a closed electronic shell, in particular Ag29-, Ag33-, and Ag39-. Both the threshol…

The influence of the trapping potential on the attachment of a second electron to stored metal cluster and fullerene anions

Abstract Singly charged anionic clusters are exposed to a bath of simultaneously stored electrons in ion cyclotron resonance (Penning) traps and thus, dianions are produced. The dianion yield is found to be a function of the potential well depth. As an example, the attachment of electrons to size-selected gold cluster anions Au 25 1− from a laser vaporization source has been studied in detail by time-of-flight mass analysis after ejection of all ions from the trap. Furthermore, the investigation is extended to fullerene anions C 70 1− that are produced by laser desorption from a fullerene target in the external source of a Fourier-transform ion cyclotron resonance (FT-ICR) mass spectrometer…

Change in structure between the $I = 1/2$ states in $^{181}$Tl and $^{177,179}$Au

Abstract The first accurate measurements of the α-decay branching ratio and half-life of the I π = 1 / 2 + ground state in 181Tl have been made, along with the first determination of the magnetic moments and I = 1 / 2 spin assignments of the ground states in 177,179Au. The results are discussed within the complementary systematics of the reduced α-decay widths and nuclear g factors of low-lying, I π = 1 / 2 + states in the neutron-deficient lead region. The findings shed light on the unexpected hindrance of the 1 / 2 + → 1 / 2 + , 181Tl → g 177 Aug α decay, which is explained by a mixing of π 3 s 1 / 2 and π 2 d 3 / 2 configurations in 177Aug, whilst 181Tlg remains a near-pure π 3 s 1 / 2 .…

The elliptical Penning trap: Experimental investigations and simulations

Abstract The application of an additional azimuthal quadrupolar electrostatic field to a Penning trap leads to a field configuration referred to as an elliptical Penning trap. The resulting changes of the radial ion motions have been investigated experimentally and by use of simulations. The eigenfrequencies, i.e., the magnetron frequency ω ˜ − and the reduced cyclotron frequency ω ˜ + , are found to be shifted with respect to those of the standard Penning trap ω − , ω + , respectively. As the shift of the magnetron frequency ω ˜ − is larger than that of the reduced cyclotron frequency ω ˜ + their sum ω ˜ + + ω ˜ − is also a function of the ellipticity and no longer equal to the cyclotron f…

Excitation and detection geometries for Fourier-transform mass spectometry

A short overview of current excitation and detection techniques for Fourier-transform mass spectrometry and related ion cyclotron resonance experiments is given, and some ideas are discussed which may lead to new developments.

Direct determination of the mass of28Si as a contribution to a new definition of the kilogram

The mass of 28Si has been determined to be m(28Si) = 27.976 926 57(30) u by comparing the cyclotron frequencies of the singly charged ions 12C+, 12C+3 and 28Si+ in a Penning trap mass spectrometer. The experimental technique and the setup are described. The obtained accuracy as well as possible improvements are discussed. Our measurements are related to current efforts to base the kilogram on atomic properties by using an almost perfect single crystal of silicon.

Phase-Imaging Ion-Cyclotron-Resonance Measurements for Short-Lived Nuclides

A novel approach based on the projection of the Penning-trap ion motion onto a position-sensitive detector opens the door to very accurate mass measurements on the ppb level even for short-lived nuclides with half-lives well below a second. In addition to the accuracy boost, the new method provides a superior resolving power by which low-lying isomeric states with excitation energy on the 10-keV level can be easily separated from the ground state. A measurement of the mass difference of ^{130}Xe and ^{129}Xe has demonstrated the great potential of the new approach.

Penning-trap mass measurements of neutron-deficient Rb and Sr isotopes

Abstract The Penning-trap mass spectrometer ISOLTRAP installed at the on-line mass separator ISOLDE 2 at CERN has been used for mass determination of 75–87 Rb and 78–83,87 Sr. Ions are captured in a Penning trap and their cyclotron frequency ω c = ( q m )B in the trapping field B is measured. Ratios of these frequencies lead to the determination of the atomic mass of these isotopes. A resolving power of typically m Δm = 10 6 and an accuracy of δm ≈10 keV is obtained. The mass of 78 Sr is measured for the first time and, in most cases, the mass values of the other isotopes are significantly improved. The experimental masses are compared with theoretical predictions.

High-Accuracy Mass Determination of Unstable Rb, Sr, Cs, Ba, Fr and Ra Isotopes with a Penning Trap Mass Spectrometer

The majority of masses of radioactive isotopes has been measured by determination of Q-values in nuclear reactions or in nuclear decay. For a long time the use of direct mass determination has been limited to stable isotopes or isotopes close to stability. This changed in the 70’s with magnetic spectrometers put on-line to isotope separators. The Orsay group (Audi et al., 1986) succeeded in measuring the masses in long isotope chains of alkali elements. They impressively demonstrated the possibilities embedded in direct mass determination of isotopes far from stability. The persisting demand for more precise masses of short-lived isotopes (or exotic particles) has prompted during recent yea…

Mass Determination of Francium and Radium Isotopes by a Penning Trap Mass Spectrometer

Abstract A tandem Penning trap mass spectrometer is used for mass measurement of radioactive isotopes produced at the on-line isotope separator ISOLDE/CERN. The mass is determined directly and with high accuracy by measuring the cyclotron frequency of the stored ions. Measurements were performed on 209 210 211 212 221 222Fr and 226 230Ra. A resolving power of 5 × 105 was used and an accuracy of 1·8 × 10−7 has been achieved.

Spectroscopy of the long-lived excited state in the neutron-deficient nuclides Po195,197,199 by precision mass measurements

Direct mass measurements of the low-spin 3/2(-) and high-spin 13/2(+) states in the neutron-deficient isotopes Po-195 and Po-197 were performed with the Penning-trap mass spectrometer ISOLTRAP at ISOLDE-CERN. These measurements allow the determination of the excitation energy of the isomeric state arising from the nu i(13/2) orbital in Po-195,Po-197. Additionally, the excitation energy of isomeric states of lead, radon, and radium isotopes in this region were obtained from alpha-decay chains. These excitation energies complete the knowledge of the energy systematics in the region and confirm that the 13/2(+) states remain isomeric, independent of the number of valence neutrons.

A penning trap for studying cluster ions

We propose to use a Penning trap for spectroscopy of stored cluster ions. A similar device has been built for the purpose of mass measurements of short-lived nuclei produced at the on-line isotope separator ISOLDE/CERN. A resolving power of 500,000 in a mass measurement of39K and an accuracy of 2 × 10−7 for the85Rb/39K mass ratio were obtained. An efficiency for in-flight capture as high as 70% was achieved. The method provides very high sensitivity since typically only 10 to 100 ions are stored in the trap. We intend to perform laser spectroscopy on trapped Na clusters as a first application of the trap technique.

High-precision Penning-trap mass measurements of heavy xenon isotopes for nuclear structure studies

With the double Penning-trap mass spectrometer ISOLTRAP at ISOLDE/CERN the masses of the neutron-rich isotopes $^{136\ensuremath{-}146}\mathrm{Xe}$ were measured with a relative uncertainty of the order of ${10}^{\ensuremath{-}8}$ to ${10}^{\ensuremath{-}7}$. In particular, the masses of $^{144\ensuremath{-}146}\mathrm{Xe}$ were measured for the first time. These new mass values allow one to extend calculations of the mass surface in this region. Proton-Neutron interaction strength, obtained from double differences of binding energies, relate to subtle structural effects, such as the onset of octupole correlations, the growth of collectivity, and its relation to the underlying shell model l…

Cluster calibration in mass spectrometry: laser desorption/ionization studies of atomic clusters and an application in precision mass spectrometry.

For accurate mass measurements and identification of atomic and molecular species precise mass calibration is mandatory. Recent studies with laser desorption/ionization and time-of-flight analysis of cluster ion production by use of fullerene and gold targets demonstrate the generation of atomic clusters for calibration purposes. Atomic ion results from the Penning trap mass spectrometer ISOLTRAP, in which a carbon cluster ion source has recently been installed, are presented as an application in the field of precision mass spectrometry.

Collision induced dissociation of doubly charged stored metal cluster ions

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 …

Excitation modes for fourier transform-ion cyclotron resonance mass spectrometry.

AbstractVarious geometric configurations for the excitation of coherent ion motion in Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICR/MS) are analyzed (in some cases for the first time) with unified notation. The instantaneous power absorption, F·v, in which v is ion velocity and F the force produced by the applied excitation electric field (harmonic, single frequency, on-resonance, in-phase), is time averaged and then set equal to the time rate of change of ion total (cyclotron + magnetron + trapping) energy, to yield a differential equation that is readily solved for the (time-dependent) amplitude of each of the various ion motions. The standard FT-ICR excitation (name…

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.

High-precision masses of neutron-deficient rubidium isotopes using a Penning trap mass spectrometer

The atomic masses of the neutron-deficient radioactive rubidium isotopes $^{74-77,79,80,83}$Rb have been measured with the Penning trap mass spectrometer ISOLTRAP. Using the time-of-flight cyclotron resonance technique, relative mass uncertainties ranging from $1.6 \times 10^{-8}$ to $5.6 \times 10^{-8}$ were achieved. In all cases, the mass precision was significantly improved as compared with the prior Atomic-Mass Evaluation; no significant deviations from the literature values were observed. The exotic nuclide $^{74}$Rb with a half-life of only 65 ms, is the shortest-lived nuclide on which a high-precision mass measurement in a Penning trap has been carried out. The significance of these…

Direct Measurement of the Mass Difference ofHo163andDy163Solves theQ-Value Puzzle for the Neutrino Mass Determination

The atomic mass difference of (163)Ho and (163)Dy has been directly measured with the Penning-trap mass spectrometer SHIPTRAP applying the novel phase-imaging ion-cyclotron-resonance technique. Our measurement has solved the long-standing problem of large discrepancies in the Q value of the electron capture in (163)Ho determined by different techniques. Our measured mass difference shifts the current Q value of 2555(16) eV evaluated in the Atomic Mass Evaluation 2012 [G. Audi et al., Chin. Phys. C 36, 1157 (2012)] by more than 7σ to 2833(30(stat))(15(sys)) eV/c(2). With the new mass difference it will be possible, e.g., to reach in the first phase of the ECHo experiment a statistical sensit…

Investigation of the magnetic field fluctuation and implementation of a temperature and pressure stabilization at SHIPTRAP

Abstract Penning traps have proven to be powerful tools for the determination of nuclear masses with high accuracy. A crucial parameter for precision mass measurements in Penning traps is the accurate determination of the magnetic-field strength. However, the magnetic field of a superconducting magnet is not constant in time, but changes due to intrinsic effects of the solenoid and external perturbations. These effects have been investigated for SHIPTRAP. Furthermore, a stabilization of the temperature in the magnet bore as well as of the pressure in the liquid-helium cryostat has been implemented. Thus, the magnetic-field related uncertainties have been reduced to 7(6)×10−11/h.

Recent Upgrades of the SHIPTRAP Setup: On the Finish Line Towards Direct Mass Spectroscopy of Superheavy Elements

With the Penning-trap mass spectrometer SHIPTRAP at GSI, Darmstadt, it is possible to investigate exotic nuclei in the region of the heaviest elements. Few years ago, challenging experiments led to the direct measurements of the masses of neutron-deficient isotopes with Z = 102,103 around N = 152. Thanks to recent advances in cooling and ion-manipulation techniques, a major technical upgrade of the setup has been recently accomplished to boost its efficiency. At present, the gap to reach more rare and shorter-lived species at the limits of the nuclear landscape has been narrowed. ispartof: pages:423-429 ispartof: Acta Physica Polonica B vol:48 issue:3 pages:423-429 ispartof: location:Zakopa…

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.

Radiative Cooling of a Small Metal Cluster: The Case ofV13+

Size-selected stored metal cluster ions, ${\mathrm{V}}_{13}^{+}$, have been heated by photoexcitation ( $\ensuremath{\lambda}\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}730$ to 229 nm) to well-defined excitation energies corresponding to temperatures between 1000 and 2100 K. A millisecond pump-probe photodissociation technique was applied to measure the time-resolved radiative cooling. The observed decay rates are directly related to the radiative energy loss and are explained quantitatively by the competing processes of photoemission and atom evaporation.

Probing cluster structures with sensor molecules: methanol adsorbed onto gold clusters

Abstract Structural, dynamical and electronic properties of the adducts formed by adsorbing methanol onto size-selected gold clusters are investigated using infrared multiple-photon dissociation spectroscopy of trapped Au n + CH 3 OH, n ⩽15, in conjunction with Car–Parrinello calculations. The C–O stretching vibration of the attached sensor molecule changes discontinuously as a function of cluster size, which is traced back to a change in dimensionality of the cluster structure.

Determination of dissociation energies by use of energy-dependent decay pathway branching ratios

Abstract We present a method for the determination of dissociation energies of polyatomic systems that undergo sequential fragmentation with energy-dependent decay pathway branching. It allows to experimentally determine the dissociation energy of any polyatomic system that shows such fragmentation behaviour without the need for a specific modelling of the system or of its fragmentation process, thus eliminating several systematic errors of traditional methods. The new method has been applied to the sequential fragmentation of Au+14 and Au+16. The resulting dissociation energies are highly accurate and in good agreement with model-free values based on rates of sequential decays.

Signature of cluster isomers in time-resolved photodissociation experiments

Abstract The unrecognized presence of structure isomers in mass-selected cluster ensembles may obstruct investigations of the systems’ intrinsic properties, since isomers differ not only in geometry, but also in other important properties. By the same token isomers are very interesting objects in the detailed study of atomic clusters. In the present work, different scenarios of isomeric coexistence are presented. They vary in the relative values of the interconversion barrier and the dissociation energies. For some idealized cases the possibility of a distinction of isomers by photodissociation experiments is discussed. In favorable situations isomeric structures may even be selected.

Shape coexistence in Au 187 studied by laser spectroscopy

Hyperfine-structure parameters and isotope shift of the 9/2$^−$ isomeric state in $^{187}$Au relative to $^{197}$Au for the 267.6-nm atomic transition have been measured for the first time using the in-source resonance-ionization spectroscopy technique. The magnetic dipole moment and change in the mean-square charge radius for this 9/2$^−$ isomer have been deduced. The observed large isomer shift relative to the 1/2$^+$ ground state in $^{187}$Au confirms the occurrence of the shape coexistence in $^{187}$Au proposed earlier from the analysis of the nuclear spectroscopic data and particle plus triaxial rotor calculations. The analysis of the magnetic moment supports the previously proposed …

Measurement and interpretation of the polarization of the x-ray line emission of heliumlike Fe XXV excited by an electron beam

The linear polarization of the 1s2p${\mathrm{}}^{1}$${\mathit{P}}_{1}$\ensuremath{\rightarrow}1${\mathit{s}}^{2}$${\mathrm{}}^{1}$${\mathit{S}}_{0}$ resonance line, the 1s2p${\mathrm{}}^{3}$${\mathit{P}}_{1,2}$\ensuremath{\rightarrow}1${\mathit{s}}^{2}$${\mathrm{}}^{1}$${\mathit{S}}_{0}$ intercombination lines, and the 1s2s${\mathrm{}}^{3}$${\mathit{S}}_{1}$\ensuremath{\rightarrow}1${\mathit{s}}^{2}$${\mathrm{}}^{1}$${\mathit{S}}_{0}$ forbidden line was measured in heliumlike Fe XXV excited near threshold by a monoenergetic electron beam. The measurement was carried out with a high-resolution x-ray spectrometer employing a set of two analyzing crystals that acted as polarizers by selectivel…

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…

Spectroscopy of short-lived radioactive molecules

Molecular spectroscopy offers opportunities for the exploration of the fundamental laws of nature and the search for new particle physics beyond the standard model1–4. Radioactive molecules—in which one or more of the atoms possesses a radioactive nucleus—can contain heavy and deformed nuclei, offering high sensitivity for investigating parity- and time-reversal-violation effects5,6. Radium monofluoride, RaF, is of particular interest because it is predicted to have an electronic structure appropriate for laser cooling6, thus paving the way for its use in high-precision spectroscopic studies. Furthermore, the effects of symmetry-violating nuclear moments are strongly enhanced5,7–9 in molecu…

The Mainz Cluster Trap

When cluster ions are stored by electromagnetic forces they are available in the gas phase for extended preparations and investigations. Over the last decade a Penning trap (Ion Cyclotron Resonance) apparatus has been constructed and further developed with respect to metal cluster research at the Institute of Physics at Mainz. It allows to capture and accumulate ion bunches injected from an external cluster source and to manipulate the ions’ motion, i.e. select and center the clusters of interest. The interactions that have been investigated include those with inert and chemically reactive gases, photons and electrons. Multiple mass spectrometric steps such as fragment ion selection can be …

Restoration of theN=82Shell Gap from Direct Mass Measurements ofSn132,134

A high-precision direct Penning trap mass measurement has revealed a 0.5-MeV deviation of the binding energy of (134)Sn from the currently accepted value. The corrected mass assignment of this neutron-rich nuclide restores the neutron-shell gap at N=82, previously considered to be a case of "shell quenching." In fact, the new shell gap value for the short-lived (132)Sn is larger than that of the doubly magic (48)Ca which is stable. The N=82 shell gap has considerable impact on fission recycling during the r process. More generally, the new finding has important consequences for microscopic mean-field theories which systematically deviate from the measured binding energies of closed-shell nu…

Mass spectrometry of atomic ions produced by in-trap decay of short-lived nuclides

The triple-trap mass spectrometer ISOLTRAP at ISOLDE/CERN has demonstrated the feasibility of mass spectrometry of in-trap-decay product ions. This novel technique gives access to radionuclides, which are not produced directly at ISOL-type radioactive ion beam facilities. As a proof of principle, the in-trap decay of $^{37}K^+$ has been investigated in a Penning trap filled with helium buffer gas. The half-life of the mother nuclide was confirmed and the recoiling $^{37}Ar^+$ daughter ion was contained within the trap. The ions of either the mother or the daughter nuclide were transferred to a precision Penning trap, where their mass was determined.

Damping effects in Penning trap mass spectrometry

Abstract Collisions of ions with residual gas atoms in a Penning trap can have a strong influence on the trajectories of the ions, depending on the atom species and the gas pressure. We report on investigations of damping effects in time-of-flight ion-cyclotron resonance mass spectrometry with the Penning trap mass spectrometers ISOLTRAP at ISOLDE/CERN (Geneva, Switzerland) and SHIPTRAP at GSI (Darmstadt, Germany). The work focuses on the interconversion of the magnetron and cyclotron motional modes, in particular the modification of the resonance profiles for quadrupolar excitation due to the damping effect of the residual gas. Extensive experiments have been performed with standard and Ra…

Trap-assisted decay spectroscopy with ISOLTRAP

Penning traps are excellent high-precision mass spectrometers for radionuclides. The high-resolving power used for cleaning isobaric and even isomeric contaminants can be exploited to improve decay-spectroscopy studies by delivering purified samples. An apparatus allowing trap-assisted decay spectroscopy has been coupled to the ISOLTRAP mass spectrometer at ISOLDE/CERN. The results from studies with stable and radioactive ions show that the setup can be used to perform decay studies on purified short-lived nuclides and to assist mass measurements. (C) 2012 Elsevier B.V. All rights reserved.

Extending Penning trap mass measurements with SHIPTRAP to the heaviest elements

Penning-trap mass spectrometry of radionuclides provides accurate mass values and absolute binding energies. Such mass measurements are sensitive indicators of the nuclear structure evolution far away from stability. Recently, direct mass measurements have been extended to the heavy elements nobelium (Z=102) and lawrencium (Z=103) with the Penning-trap mass spectrometer SHIPTRAP. The results probe nuclear shell effects at N=152. New developments will pave the way to access even heavier nuclides.

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…

Mass Measurements of Very Neutron-Deficient Mo and Tc Isotopes and Their Impact on rp Process Nucleosynthesis

The masses of ten proton-rich nuclides, including the N=Z+1 nuclides 85-Mo and 87-Tc, were measured with the Penning trap mass spectrometer SHIPTRAP. Compared to the Atomic Mass Evaluation 2003 a systematic shift of the mass surface by up to 1.6 MeV is observed causing significant abundance changes of the ashes of astrophysical X-ray bursts. Surprisingly low alpha-separation energies for neutron-deficient Mo and Tc are found, making the formation of a ZrNb cycle in the rp process possible. Such a cycle would impose an upper temperature limit for the synthesis of elements beyond Nb in the rp process.

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.

The performance of the cryogenic buffer-gas stopping cell of SHIPTRAP

Direct high-precision mass spectrometry of the heaviest elements with SHIPTRAP, at GSI in Darmstadt, Germany, requires high efficiency to deal with the low production rates of such exotic nuclides. A second-generation gas stopping cell, operating at cryogenic temperatures, was developed and recently integrated into the relocated system to boost the overall efficiency. Offline measurements using 223Ra and 225Ac recoil-ion sources placed inside the gas volume were performed to characterize the gas stopping cell with respect to purity and extraction efficiency. In addition, a first online test using the fusion-evaporation residue 254No was performed, resulting in a combined stopping and extrac…

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.

Direct Mapping of Nuclear Shell Effects in the Heaviest Elements

Quantum-mechanical shell effects are expected to strongly enhance nuclear binding on an "island of stability" of superheavy elements. The predicted center at proton number $Z=114,120$, or $126$ and neutron number $N=184$ has been substantiated by the recent synthesis of new elements up to $Z=118$. However the location of the center and the extension of the island of stability remain vague. High-precision mass spectrometry allows the direct measurement of nuclear binding energies and thus the determination of the strength of shell effects. Here, we present such measurements for nobelium and lawrencium isotopes, which also pin down the deformed shell gap at $N=152$.

High-accuracy mass measurements of neutron-rich Kr isotopes

The atomic masses of the neutron-rich krypton isotopes {sup 84,86-95}Kr have been determined with the tandem Penning trap mass spectrometer ISOLTRAP with uncertainties ranging from 20 to 220 ppb. The masses of the short-lived isotopes {sup 94}Kr and {sup 95}Kr were measured for the first time. The masses of the radioactive nuclides {sup 89}Kr and {sup 91}Kr disagree by 4 and 6 standard deviations, respectively, from the present Atomic-Mass Evaluation database. The resulting modification of the mass surface with respect to the two-neutron separation energies as well as implications for mass models and stellar nucleosynthesis are discussed.

Accurate mass determination of short-lived isotopes by a tandem Penning-trap mass spectrometer

A mass spectrometer consisting of two Penning traps has been set up for short-lived isotopes at the on-line mass separator ISOLDE at CERN. The ion beam is collected and cooled in the first trap. After delivery to the second trap, high-accuracy direct mass measurements are made by determining the cyclotron frequency of the stored ions. Measurements have been performed for $^{118}--^{137}$Cs. A resolving power of over ${10}^{6}$ and an accuracy of 1.4\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}7}$ have been achieved, corresponding to about 20 keV.

Recent gold cluster studies in a Penning trap

Abstract A progress report is given on the investigation of metal clusters with an ion cyclotron resonance (Penning) trap. The examples are taken from the recent studies on gold clusters. In particular, the monomer and dimer evaporation is monitored as a function of cluster size. For the particular case of Au 7 + this study is expanded to include the energy dependence of the branching ratio. In connection with the sequential decay of Au 8 + the information can be used for a model-free determination of the dissociation energy of Au 8 + . A second line of studies concerns the production, properties and storage behavior of polyanionic gold clusters. Such species have recently been produced by …

Photoinduced dissociation of anionic and electron detachment of dianionic gold clusters by use of a laser pointer

Abstract Size-selected anionic and dianionic gold clusters have been stored in a Penning trap and irradiated with the green light of a laser pointer. As examples of special interest, the systems Au 7 − and Au 29 2− have been chosen. In particular, Au 7 − , a small gold cluster with closed electron shell, is observed to decay into Au 6 − and Au 5 − with a decay pathway branching ratio similar to that of Au 9 + . The dianionic cluster Au 29 2− shows electron detachment upon photoexcitation. This observation is in agreement with independent experiments [Stoermer et al., Int. J. Mass Spectrom. 201 (2001) 63], where Au 29 2− is found to be the smallest dianion produced by neutral monomer evapora…

Production of dianionic and trianionic noble metal clusters in a Penning trap

Abstract Metal clusters, Aun−, Agn−, and Cun−, from a laser vaporization source are transferred to a Penning trap and subjected to a bath of simultaneously stored electrons. After some reaction period multiply charged anionic gold, silver, and copper clusters are observed if the clusters under investigation are large enough. The cluster sizes for the onset of the formation of dianions and trianions are compared to a charged sphere model. The description of the experimental findings is largely improved if the repulsive Coulomb barrier is taken into account which prevents autodetachment of the surplus electrons on the experimental time scale of a second.

Decay pathways of stored metal-cluster anions after collisional activation

Size-selected gold clusters, Open image in new window (n ≤ 21), and tungsten clusters, Open image in new window , and Open image in new window (n = 4 – 8 and 12), stored in a Penning trap have been collisionally activated. Neutral monomer and dimer evaporation are observed in the case of gold. While no fragment products have been observed for tungsten clusters, there is evidence of electron emission from the anions.

Charge radii and electromagnetic moments of At195–211

Hyperfine-structure parameters and isotope shifts of At195-211 have been measured for the first time at CERN-ISOLDE, using the in-source resonance-ionization spectroscopy method. The hyperfine structures of isotopes were recorded using a triad of experimental techniques for monitoring the photo-ion current. The Multi-Reflection Time-of-Flight Mass Spectrometer, in connection with a high-resolution electron multiplier, was used as an ion-counting setup for isotopes that either were affected by strong isobaric contamination or possessed a long half-life; the ISOLDE Faraday cups were used for cases with high-intensity beams; and the Windmill decay station was used for short-lived, predominantl…

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+ .

X-ray measurements of charge transfer reactions involving cold, very highly charged ions

The magnetic trapping mode of the Livermore high-energy Electron Beam Ion Trap is exploited to study charge transfer reactions between cold (few eV/amu) highly charged ions and gases. By selectively puffing neutral gases and monitoring the x-ray emission, state-selective measurements of the charge transfer reaction channels are possible. The observed K-shell x-ray spectra show prominent emission from high-n levels decaying to the n = 1 ground level, which is enabled by electron capture into states with low orbital angular momentum. A comparison with modeling calculations, therefore, allows a determination of the range of principal and angular momentum quantum numbers involved in the reactio…

First Observation of Doubly Charged Negative Gold Cluster Ions

Singly charged gold cluster anions in the size range n = 16–30 have been captured, stored and size selected in a Penning trap. After application of an electron beam doubly charged gold cluster anions have been observed for 20 ≤ n ≤ 30. To our knowledge this is the first observation of metal cluster dianions. The threshold appearance size is in good agreement with a simple charged sphere model. The application of argon gas pulses simultaneously with the electron beam is found to increase the production rate by an order of magnitude.

ISOLTRAP Mass Measurements for Weak-Interaction Studies

International audience; The conserved-vector-current (CVC) hypothesis of the weak interaction and the unitarity of the Cabibbo-Kobayashi-Maskawa (CKM) matrix are two fundamental postulates of the Standard Model. While existing data on CVC supports vector current conservation, the unitarity test of the CKM matrix currently fails by more than two standard deviations. High-precision mass measurements performed with the ISOLTRAP experiment at ISOLDE/CERN provide crucial input for these fundamental studies by greatly improving our knowledge of the decay energy of super-allowed beta decays. Recent results of mass measurements on the beta emitters 18Ne, 22Mg, 34Ar, and 74Rb as pertaining to weak-i…

Characterization of the shape-staggering effect in mercury nuclei

In rare cases, the removal of a single proton (Z) or neutron (N) from an atomic nucleus leads to a dramatic shape change. These instances are crucial for understanding the components of the nuclear interactions that drive deformation. The mercury isotopes (Z = 80) are a striking example1,2: their close neighbours, the lead isotopes (Z = 82), are spherical and steadily shrink with decreasing N. The even-mass (A = N + Z) mercury isotopes follow this trend. The odd-mass mercury isotopes 181,183,185Hg, however, exhibit noticeably larger charge radii. Due to the experimental difficulties of probing extremely neutron-deficient systems, and the computational complexity of modelling such heavy nucl…

Energy dependence of the decay pathways of optically excited small gold clusters

The pathway competition between neutral monomer and neutral dimer evaporation from optically excited odd-size gold cluster ions Au+ n, n=7–15, has been investigated as a function of cluster size and excitation energy. Gold cluster ions of these sizes are the only ones to show observable pathway competition while all other sizes exclusively evaporate either neutral monomers or neutral dimers. The investigation has been performed by photoexcitation of stored size-selected gold cluster ions with a single 10-ns laser pulse. Subsequent time-resolved observation of the delayed dissociation allows us to quantitatively determine the relative fragment yields of the respective decay channels as a fun…

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.

Dimer dissociation energies of small odd-size clusters

The dimer dissociation energies of gold cluster ions Au + n , n = 9, 11, 13, 15 have been determined with an extension of a recently developed model-independent method. Monomer-dimer decay pathway branching ratios provide the energy dependent process which is needed in this method. The measured values are D 2 ( Au + 9 ) = 3.66(8)(9) eV, D 2 ( Au + 11 ) = 4.27(11)(8) eV, D 2 ( Au + 13 ) = 4.50(9)(7) eV and D 2 ( Au + 15 ) = 4.29(10)(6) eV.

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…

High-accuracy mass measurements on neutron deficient neon isotopes

International audience; The atomic masses of the short-lived nuclides 17Ne and 19Ne have been measured with the triple-trap mass spectrometer ISOLTRAP at ISOLDE/CERN. The obtained mass excess for both nuclides deviates significantly from the literature value, in the case of 17Ne about 40 keV. The mass value of 17Ne can be applied for a test of the isobaric multiplet mass equation with respect to an isospin T = 3/2 quartet. In addition, both masses can contribute to the data analysis of collinear laser-spectroscopy experiments where mean-square nuclear-charge radii are determined.

FT-ICR MS studies of ion-molecule reactions of Ru+ and Os+ with oxygen

Abstract The reactions of stored ruthenium and osmium cations with oxygen have been studied in a Fourier transform ion cyclotron resonance (FT-ICR) mass spectrometer. In case of osmium the reaction products OsO+ and OsO 2 + have been observed and corresponding reaction-rate constants have been determined. In addition, there is an unreactive fraction of Os+ ions due to the presence of a slightly endothermic reacting ground state. Only the excited states react with oxygen. For ruthenium no spontaneous reaction with oxygen has been observed unless the cyclotron motion of Ru+ was excited. The results are discussed with respect to a similar investigation in a Penning trap-TOF mass spectrometer […

Mass measurements of $^{56-57}$Cr and the question of shell reincarnation at N = 32

Binding energies determined with high accuracy provide smooth derivatives of the mass surface for analysis of shell and pairing effects. Measurements with the Penning trap mass spectrometer ISOLTRAP at CERN-ISOLDE were made for $^{56-57}$Cr for which an accuracy of 4 $\times 10^{-8}$ was achieved. Analysis of the mass surface for the supposed new N = 32 shell closure rather indicates a sub-shell closure, but of a different nature than known cases such as $^{94}$Sr.