Improvement of the Applicability, Efficiency, andPrecision of the Penning Trap Mass Spectrometer ISOLTRAP

With the Penning trap mass spectrometer ISOLTRAP, close to 200 nuclides have already been investigated and their masses determined with a typical relative precision of δm/m=10⁻⁷. Recently, ISOLTRAP's beam preparation system was replaced by an RFQ ion beam cooler and buncher. The principle and the characteristics of this new beam preparation system will be presented. It is planned to use ions of various carbon clusters C⁺ _n (n>1) as reference ions for mass measurements. Apart from negligible molecular binding energies, these clusters have masses that are exact multiples of the unified atomic mass unit. This will allow ISOLTRAP to carry out absolute mass measurements as well as to investigate possible mass-dependent systematic errors. The results of tests of the production, transport, and trapping of such carbon clusters will be presented. This revised version was published online in July 2006 with corrections to the Cover Date.     

From direct to absolute mass measurements: A study of the accuracy of ISOLTRAP

For a detailed study of the accuracy of the Penning trap mass spectrometer ISOLTRAP all expected sources of uncertainty were investigated with respect to their contributions to the uncertainty of the final result. In the course of these investigations, cross-reference measurements with singly charged carbon clusters ¹²C⁺ _n were carried out. The carbon cluster ions were produced by use of laser-induced desorption, fragmentation, and ionization of C₆₀ fullerenes and injected into and stored in the Penning trap system. The comparison of the cyclotron frequencies of different carbon clusters has provided detailed insight into the residual systematic uncertainty of ISOLTRAP and yielded a value of 8×10^-9. This also represents the current limit of mass accuracy of the apparatus. Since the unified atomic mass unit is defined as 1/12 of the mass of the ¹²C atom, it will be possible to carry out absolute mass measurements with ISOLTRAP in the future. Received 7 June 2002 Published online 6 November 2002 RID="a" ID="a"e-mail: a.kellerbauer@cern.ch RID="b" ID="b"Current address: Centre de Physique des Particules de Marseille, 13288 Marseille Cedex 9, France.     

Accurate mass measurements of very short-lived nuclei

Mass measurements of ³⁴Ar, ^73-78Kr, and ^74,76Rb were performed with the Penning-trap mass spectrometer ISOLTRAP. Very accurate Q _EC-values are needed for the investigations of the t-value of 0⁺ → 0⁺ nuclear β-decays used to test the standard model predictions for weak interactions. The necessary accuracy on the Q _EC-value requires the mass of mother and daughter nuclei to be measured with δm/m ⩽ 3 ^. 10^-8. For most of the measured nuclides presented here this has been reached. The ³⁴Ar mass has been measured with a relative accuracy of 1.1 ^. 10^-8. The Q _EC-value of the ³⁴Ar 0⁺ → 0⁺ decay can now be determined with an uncertainty of about 0.01%. Furthermore, ⁷⁴Rb is the shortest-lived nuclide ever investigated in a Penning trap. Received: 21 March 2002 / Accepted: 16 May 2002 / Published online: 31 October 2002 RID="a" ID="a"e-mail: frank.herfurth@cern.ch     

Laser Ionization and Penning Trap Mass Spectrometry – A Fruitful Combination for Isomer Separation and High-precision Mass Measurements

We have demonstrated for the first time that element-selective laser ionization in combination with ultra-high resolution mass spectrometry can be used to prepare isomerically pure ion ensembles. Together with β–γ coincidence studies this method allowed a determination of the low-energy structure and the unambiguous identification of triple β-decaying isomerism in ⁷⁰Cu. By selective resonant ionization and measurement of the masses of these three states using ISOLTRAP at ISOLDE/CERN with a relative uncertainty of δm/m ≈ 5 ⋅ 10⁻⁸ a clear state-to-mass assignment was possible which resolved the assignment puzzle in ⁷⁰Cu.     

Selective laser ionization of N≥82 indium isotopes: The new r-process nuclide 135In

Production yields and β-decay half-lives (T _1/2) of very neutron-rich indium isotopes were determined at CERN/ISOLDE using isobaric selectivity of a resonance-ionization laser ion-source. Beta-delayed neutron (βdn) multiscaling measurements have yielded improved T _1/2 for 206(6) ms ¹³²In, 165(3) ms ¹³³In and 141(5) ms ¹³⁴In. With 92(10) ms ¹³⁵In, a new r-process nuclide has been identified which acts as an important “waiting point” in the In isotopic chain for neutron densities in the range n _n≃ 10²⁴-10²⁶ n/cm³, where the r-matter flow has already passed the A≃ 130 abundance peak region. Received: 17 January 2002 / Accepted: 30 January 2002     

ISOLTRAP: A tandem penning trap mass spectrometer for radioactive isotopes

The masses of over sixty short-lived Rb, Sr, Cs, Ba, Fr and Ra isotopes have been measured at the on-line mass separator ISOLDE at CERN/Geneva by determination of their cyclotron frequency in the tandem Penning trap system ISOLTRAP. Resolving powers exceedingm/m(FWHM)=10⁶ and accuracies of typically m/m=10^–7 could be achieved. ISOLTRAP can also act as an isomer separator, as proven for the cases of⁸⁴Rb and⁷⁸Rb.     

Mass Measurements of 114–124,130Xe with the ISOLTRAP Penning Trap Spectrometer

The masses of the xenon isotopes with 114≤A≤123 were directly measured for the first time. The experiments were carried out at the ISOLTRAP triple trap spectrometer at the on-line mass separator ISOLDE/CERN. A mass resolving power of the Penning trap spectrometer of m/Δm≈500 000 was chosen and an accuracy of δm≈12keV for all investigated Xe isotopes was achieved. An atomic mass evaluation was performed and the results of this adjustment are compared with theoretical predictions. The new results for the xenon isotopes and their effects on neighboring nuclides are discussed within the two-neutron separation energy picture. This revised version was published online in July 2006 with corrections to the Cover Date.     

Charge radius change in the heavy tin isotopes until A = 132 from laser spectroscopy

Laser spectroscopy measurements have been carried out on the very neutron-rich tin isotopes with the COMPLIS experimental setup. Using the 5s ²5p ²³ P ₀ → 5s ²5p6s ³ P ₁ optical transition, hyperfine spectra of ^126-132Sn and ^{125m, 127m, 129m-131m}Sn where recorded for the first time. The variation of the mean-square charge radius ( δ〈r ²〉) between these nuclei and nuclear moments of the isomers and the odd isotopes were thus measured. An odd-even staggering which inverts at A = 130 is clearly observed. This indicates a small appearance of a plateau on the δ〈r ²〉 which has to be confirmed by measuring the isotope shift beyond A = 132. Received: 21 March 2002 / Accepted: 16 May 2002 / Published online: 31 October 2002 RID="a" ID="a"e-mail: leblanc@ipno.in2p3.fr     

Charge distribution studies in the fast-neutron-induced fission of <Superscript>232</Superscript>Th, <Superscript>238</Superscript>U, <Superscript>240</Superscript>Pu and <Superscript>244</Superscript>Cm

Charge distribution studies for heavy-mass fission products were carried out in the fast-neutron-induced fission of ²³²Th, ²³⁸U, ²⁴⁰Pu and ²⁴⁴Cm using radiochemical and gamma-ray spectrometric techniques. The width parameter( σ_Z/σ_A), the most probable charge/mass ( Z _P/A _P), the charge polarization (ΔZ) and the slope of charge polarization [ δ(ΔZ)/δA ^′] as a function of the fragment mass (A ^′) were deduced. The average charge dispersion parameter ( 〈σ_Z〉) and proton odd-even effect ( δ_p) were also obtained for these fissioning systems. The 〈σ_Z〉 and δ_p values in the fissioning systems ²⁴¹Pu ^* and ²⁴⁵Cm ^* were determined for the first time. The δ(ΔZ)/δA ^′ value is also determined for the first time in the fissioning systems ²³⁹U ^* , ²⁴¹Pu ^* and ²⁴⁵Cm ^* . These data along with the literature data for even-Z fissioning systems such as ²³⁰Th ^* , ²³²Th ^* , ²³³U ^* , ²³⁴U ^* , ²³⁶U ^* , ²³⁸U ^* , ²³⁹Pu ^* , ²⁴⁰Pu*, ²⁴²Pu ^* , ²⁴⁶Cm ^* , ²⁵⁰Cf ^* and ²⁵²Cf(SF) are discussed in terms of nuclear structure effect and dynamics of descent from the saddle to the scission point. The role of the excitation energy in low-energy fission is also discussed. Received: 26 July 2002 / Accepted: 3 December 2002 / Published online: 3 April 2003 RID="a" ID="a"Present address: Emeritus Scientist (CSIR) Bhabha Atomic Research Centre, Nuclear Recycle Group, WIP Building, Trombay, Mumbai-400085, India; e-mail: rhiyer@magnum. barc.ernet.in Communicated by D. Schwalm     

Accurate masses of unstable rare-earth isotopes by ISOLTRAP

Direct mass measurements of neutron-deficient rare-earth isotopes in the vicinity of ¹⁴⁶Gd were performed with the Penning trap mass spectrometer ISOLTRAP at ISOLDE/CERN. This paper reports on the measurement of more than 40 isotopes of the elements praseodymium, neodymium, promethium, samarium, europium, dysprosium and holmium, that have been measured with a typical accuracy of m 14 keV. An atomic mass evaluation has been performed taking into account other experimental mass values via a least-squares adjustment. The results of the adjustment are discussed. Received: 18 April 2000 / Accepted: 12 July 2000     

SiC bonding in ( C 60 ) n Si m clusters

This paper deals with a new type of SiC bonding where silicon atom seems to bridge C₆₀ molecules. We have studied films obtained by deposition of (C₆₀)_nSi_m clusters prepared in a laser vaporization source. Prior deposition, free ionized clusters were studied in a time-of-flight mass spectrometer. Mixed clusters (C₆₀)_nSi_m were clearly observed. Abundance and photofragmentation mass spectroscopies revealed the relatively high stability of the (C₆₀)_nSi _n ⁺ , (C₆₀)_nSi _{n - 1} ⁺ and (C₆₀)_nSi _{n - 2} ⁺ species. This observation is in favor of the arrangement of these complexes as polymers where the C₆₀ cages may be bridged by a silicon atom. Free neutral clusters are then deposited onto substrate making up a nanogranular thin film (≃ 100 nm). The film is probed by Auger and X-ray photoemission spectroscopies, but above all by surface enhanced Raman scattering. The results suggest an unusual chemical bonding between silicon and carbon and the environment of the silicon atom is expected to be totally different from the sp³ lattice: ten or twelve carbon neighbors might surround silicon atom. The bonding is discussed to the light of the so-called fullerene polymerization as observed for pure fullerite upon laser irradiation. This opens a new route for bridging C₆₀ molecules together with an appreciable energy bonding, since the usual van der Waals bonding in fullerite could be replaced by an ionocovalent bond. Such an assumption must be checked in the future by XAS and EXAFS experiments. Received 15 November 2000     

Generation of CdS clusters using laser ablation: the role of wavelength and fluence

The formation of cationic clusters in the laser ablation of CdS targets has been investigated as a function of wavelength and fluence by mass spectrometric analysis of the plume. Ablation was carried out at the laser wavelengths of 1064, 532, 355, and 266 nm in order to scan the interaction regimes below and above the energy band gap of the material. In all cases, the mass spectra showed stoichiometric Cd _n S _n ⁺ and nonstoichiometric Cd _n S _n−1⁺, Cd _n S _n+1⁺, and Cd _n S _n+2⁺ clusters up to 4900 amu. Cluster size distributions were well represented by a log-normal function, although larger relative abundance for clusters with n=13, 16, 19, 34 was observed (magic numbers). The laser threshold fluence for cluster observation was strongly dependent on wavelength, ranging from around 16 mJ/cm² at 266 nm to more than 300 mJ/cm² at 532 and 1064 nm. According to the behavior of the detected species as a function of fluence, two distinct families were identified: the “light” family containing S₂⁺ and Cd⁺ and the “heavy” clusterized family grouping Cd₂⁺ and Cd _n S _m ⁺. In terms of fluence, it has been determined that the best ratio for clusterization is achieved close to the threshold of appearance of clusters at all wavelengths. At 1064, 532, and 355 nm, the production of “heavy” cations as a function of fluence showed a maximum, indicating the participation of competitive effects, whereas saturation is observed at 266 nm. In terms of relative production, the contribution of the “heavy” family to the total cation signal was significantly lower for 266 nm than for the longer wavelengths. Irradiation at 355 nm in the fluence region of 200 mJ/cm² has been identified as the optimum for the generation of large clusters in CdS.     

The Z = 82 shell closure in neutron-deficient Pb isotopes

Recent mass measurements show a substantial weakening of the binding-energy difference δ_2p(Z, N) = E(Z - 2, N) - 2E(Z, N) + E(Z + 2, N) in the neutron-deficient Pb isotopes. As δ_2p is often attributed to the size of the proton magic gap, it might be speculated that reduction in δ_2p is related to a weakening of the spherical Z = 82 shell. We demonstrate that the observed trend is described quantitatively by self-consistent mean-field models in terms of deformed ground states of Hg and Po isotopes. Received: 25 October 2001 / Accepted: 28 February 2002     

ISOLTRAP: An on-line Penning trap for mass spectrometry on short-lived nuclides

ISOLTRAP is a Penning trap mass spectrometer for high-precision mass measurements on short-lived nuclides installed at the on-line isotope separator ISOLDE at CERN. The masses of close to 300 radionuclides have been determined up to now. The applicability of Penning trap mass spectrometry to mass measurements of exotic nuclei has been extended considerably at ISOLTRAP by improving and developing this double Penning trap mass spectrometer over the past two decades. The accurate determination of nuclear binding energies far from stability includes nuclei that are produced at rates less than 100 ions/s and with half-lives well below 100ms. The mass-resolving power reaches 10⁷ corresponding to 10keV for medium heavy nuclei and the uncertainty of the resulting mass values has been pushed down to below 10^-8. The article describes technical developments achieved since 1996 and the present performance of ISOLTRAP.     

Solvation and chemical reaction of sodium in water clusters

Na_m(H₂O)_n Clusters ( n = 1...200, m = 1...50) are formed in a recently build pick-up arrangement. Preformed water clusters traverse a sodium oven, where sodium atoms are picked up. At low sodium vapour pressure ( < 1×10^-4 mbar) pure Na(H₂O)_n clusters are observed in the mass spectra. At high sodium vapour pressure ( > 1×10^-3 mbar) the water cluster pick up more than 50 Na atoms and reaction products Na(NaOH)_n ( n = 2, 4...50) dominate the mass spectra. The even number of NaOH units in the products indicate that also in a finite cluster the reaction occurs in pairs as in the macroscopic reaction. Received 4 December 2000     

Hydrogenated carbon clusters produced by highly charged ion impact on solid

The emission of small (hydrogenated) carbon cluster ions C_nHm ⁺ (n =2-22) upon highly charged Xe^q+ (q =20-44) impact on C₈₄ surfaces is studied by means of time-of-flight secondary ion mass spectrometry. The respective stage of hydrogenation/protonation of a certain carbon cluster ion Cn ⁺ is a strong indication for its geometrical structure. From the cluster ion yield as a function of cluster size it can be concluded, that the hydrogenation takes place after the initial carbon cluster formation. The carbon clusters seem to be emitted as an entity in agreement with “equilibrium” and “shock wave” models. Received 4 February 2000     

Photoacoustic gas sensing employing fundamental and frequency-doubled radiation of a continuously tunable high-pressure CO2 laser

We present the first photoacoustic spectrometer for gas sensing employing both the fundamental and the frequency-doubled radiation of a continuously tunable high-pressure CO₂ laser with room temperature operation. A quasi-phase-matched diffusion-bonded GaAs crystal is used in the system for second-harmonic generation. A pulsed photoacoustic detection scheme with a non-resonant cell, equipped with an 80-microphone array, is employed. The wide continuous tuning range in the fundamental (9.2–10.7 μm) and the frequency-doubled (4.6–5.35 μm) regimes, together with the narrow linewidth of 540 MHz (0.018 cm^-1) for the 10-μm region and of 1050 MHz (0.0315 cm^-1) for the 5-μm region, allow the measurement of gas mixtures, individual species and isotope discrimination. This is illustrated with measurements on NO and CO₂. The measured isotope ratio ¹⁵ NO/¹⁴ NO=(3.58±0.55)×10^-3 agrees well with the literature (3.700×10^-3) and demonstrates the good selectivity of the system. Received: 30 April 2002 / Revised version: 10 June 2002 / Published online: 2 September 2002 RID="*" ID="*"Corresponding author. Fax: +41-1/633-1077, E-mail: sigrist@iqe.phys.ethz.ch     

Carbon-cluster mass calibration at SHIPTRAP

A carbon-cluster ion source has been installed and tested at SHIPTRAP, the Penning-trap mass spectrometer for precision mass measurements of heavy elements at GSI. Carbon-cluster ions ¹²C_n ⁺, 5 ≤n ≤23, were produced by laser-induced desorption and ionization from a carbon sample. They were tested for the first time as reference ions in an on-line mass measurement of the radionuclides ¹⁴⁴Dy, ¹⁴⁶Dy and ¹⁴⁷Ho. In addition, carbon clusters of various sizes were used for an investigation of the systematic uncertainty of SHIPTRAP covering a mass range from 84 u to 240 u. The mass-dependent uncertainty was found to be negligible for the case of (m-m _ref)< 100 u. However, a systematic uncertainty of 4.5 ×10^-8 was revealed.     

Thermodynamic properties of the most stable gaseous small silicon-carbon clusters in their ground states

The most stable structures of gaseous Si _m C _n (3 ⩽ n+m ⩽ 6) clusters in their ground electronic states are determined with the high level electronic correlation method QCISD(T)/g3large. Thermodynamic properties on heat capacity (C _p,m ^Θ), entropy (S _m ^Θ), Gibbs energy function (−[G ^Θ −H ^Θ(T _r )]/T) and enthalpy function (H ^Θ−H ^Θ(T _r )) are predicted with standard statistical thermodynamics using the structure parameters and vibrational frequencies obtained with B3PW91/6-31G(d) method combined with the electronic excitation energies determined with time dependent density functional (TD DFT) method at B3PW91/6-31G(d) level. The electronic energies are calculated with the accurate model chemistry method at G3(QCI) level of theory and the Δ _f H _m ^Θ (0 K), Δ _f H _m ^Θ (298.15 K) and Δ _f G _m ^Θ (298.15 K) values are predicted. The heat capacities C _p,m ^Θ(T) as a function of temperature within 298.15-2000 K are fitted into analytical equations. The thermodynamic functions at higher temperatures are determined classically by using these equations. Most of the results obtained in this work are consistent with the available experiments.     

Continuum light emission from sputtered species of graphite during ion beam irradiation

Light emission during sputtering of graphite targets with 1–10 keV Ne⁺, Kr⁺ and Xe⁺ beams has been investigated in the 180-600 nm wavelength range. Beside the characteristic lines of sputtered C₁ and C₁ ⁺, a continuum superimposed with a number of broad structures was observed in the 250-520 nm range, and having a maximum at 386 nm. Mass analysis of the sputtered flux confirmed the presence of negative carbon clusters C _m ^- , C₂ ^- being the dominant one. Ion beam parameters i.e. ion mass, energy, current density and ion dose were varied to identify the origin of the continuum emission. On the basis of the experimental results, it is suggested that the continuum is predominantly due to the overlapping of various band systems of sputtered C₂ with a small contribution from the heavier sputtered carbon clusters C_m (m>2). Received 24 September 1999 and Received in final form 11 February 2000