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Ru isotopic compositions of magmatic iron meteorites and chondrites overlap with terrestrial Ru at the 0.3 to 0.9 (epsilon) level. Additional information is contained in the original extended abstract.
The breaking of axial symmetry in nuclei enables otherwise precluded behaviours, making it an interesting phenomenon to study. Experimental fingerprints such as very low-lying $2^+_2$ states suggest pronounced triaxial deformation for the neutron-rich ruthenium isotopes. Nevertheless, theoretical calculations differ in the description of the triaxial deformation and its evolution with neutron number, making experimental data crucial to understanding it. We investigated the evolution of the degree of triaxiality and $γ$ rigidity in neutron-rich ruthenium isotopes by measuring lifetimes of excited states in 108-112 Ru with the recoil distance Doppler-shift method. The experiment was carried out at the Grand Accélérateur National d’Ions Lourds using the Advanced Gamma Tracking Array coupled to the Variable Mode Spectrometer. We obtained B(E2) values for 29 transitions in the studied nuclei and compared them with fully microscopic symmetry conserving configuration mixing calculations, and phenomenological generalized triaxial rotor and triaxial particle-rotor models. The models generally reproduce the measured transition strengths, and show an increase in triaxiality with neutron number, reaching near maximum triaxiality in 112 Ru. The results are consistent with a transition from soft to rigid motion as the neutron number increases.
Nuclear structure data pertaining to all nuclei with mass number A=93 (Se, Br, Kr, Rb, Sr, Y, Zr, Nb, Mo, Tc, Ru, Rh, Pd, Ag) have been compiled and evaluated and incorporated into the ENSDF data file. This publication for A=93 supersedes the previous publication by C.M. Baglin, Nuclear Data Sheets80, 1 (1997) (literature cutoff date November 1996) and subsequent revisions by C.M. Baglin of the ENSDF files for 93Br and {sup 93}Kr (literature cutoff 26 February 2001) and for {sup 93}Rh (literature cutoff 27 February 2001); it includes all data available prior to 15 December 2010. Significant changes since prior evaluations include the following: 2010Hw03 identified several high-spin states in {sup 93}Kr in {sup 252}Cf SF decay; in addition to the many low-spin levels already known in {sup 93}Rb from {beta}{sup -} decay, several higher-spin states have now been identified in a {sup 252}Cf SF decay study (2009Hw03); this SF decay has also been used to identify additional states in {sup 93}Sr (2003Hw01) and the {sup 238}U({sup 82}Se,X{gamma}) reaction (2007Bu35) has provided new information on {sup 93}Y. (HI,xn{gamma}) reaction studies have expanded our knowledge of the structure of {sup 93}Zr (2002Fo03, 2005Pa48), {sup 93}Nb (2007Wa45), {sup 93}Mo (2005Fu01), {sup 93}Tc (2003Ha22) and {sup 93}Pd (2004So04,2004Ru02). Considerable information on {sup 93}Nb was provided by a (p,2n{gamma}) study (2010Or01, 2006Or09, 2007Or01). The level schemes of {sup 93}Ru, {sup 93}Rh and {sup 93}Pd have undergone the most extensive revision thanks to studies of {sup 93}Rh {epsilon} decay (2004De40), {sup 94}Ag {epsilon}p decay (2004Mu30) and {sup 94}Ag p decay (2005Mu15, 2005Mu30), respectively. The half-life of the Zr member of this chain is of particular interest because of {sup 93}Zr's large contribution to long-term activity of nuclear reactor waste and also due to its potential as a supernova chronometer. During 2010, two new well-documented measurements of T{sub 1/2}({sup 93}Zr) were published (2010Ya01 and 2010Ca01); one agrees well with an earlier, undocumented measurement but, unfortunately, the other is many standard deviations lower for reasons which are not immediately apparent.
This study demonstrates a new method of radioisotope labeling of ultra-high molecular weight polyethylene inserts in prosthetic joints for wear studies. The radioisotopes {sup 97}Ru, {sup 100}Pd, {sup 100}Rh, and {sup 101m}Rh are produced in fusion evaporation reactions induced by {sup 12}C ions in a {sup 92}Zr target foil. The fusion products recoil-implant into ultra-high molecular weight polyethylene plugs, machined to fit into the surface of the inserts. During laboratory simulations of the joint motion, a wear rate of the labeled polyethylene may be measured and the pathways of wear debris particles can be traced by detecting characteristic gamma-rays. The concentration profiles of the radioisotopes extend effectively uniformly from the polyethylene surface to a depth of about 4 {mu}m. The multiplicity of labeling and the use of several gamma-ray lines aids with avoiding systematic measurement uncertainties. Two polyethylene plugs were labeled and one was fitted into the surface of the tibial insert of a knee prosthesis, which had been worn in. Actuation over close to 100,000 cycles with a 900 N axial load and a 24 deg. flexion angle removed (14{+-}1)% of the gamma-ray activity from the plug. Most of this activity dispersed into the serum lubricant identifying this as the important debris pathway. Less than 1% activity was transferred to the femoral component of the prosthesis and the measured activity on the tibial tray was insignificant. Assuming uniform wear across the superior surface of the insert, a wear rate of (12{+-}3) mm{sup 3}/Megacycle was determined. This is consistent with wear rate measurements under similar conditions using other techniques.
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This article presents a method for destructive analysis of irradiated uranium (U) targets, with a focus on collection and measurement of long-lived (t 1/2 > ~10 years) and stable fission product isotopes of ruthenium and cesium. Long-lived and stable isotopes of these elements can provide information on reactor conditions (e.g. flux, irradiation time, cooling time) in old samples (> 5–10 years) whose short-lived fission products have decayed away. The separation and analytical procedures were tested on archived U reactor targets at Los Alamos National Laboratory as part of an effort to evaluate reactor models at low-burnup.
Experimentally measured isotopic concentrations of well characterized spent nuclear fuel (SNF) samples have been collected and analyzed by previous researchers. These sets of experimental data have been used extensively to validate the accuracy of depletion code predictions for given sets of burnups, initial enrichments, and varying power histories for different reactor types. The purpose of this report is to present the diversity of data in a concise manner and summarize the current accuracy of depletion modeling. All calculations performed for this report were done using the Oak Ridge Isotope GENeration (ORIGEN) code, an internationally used irradiation and decay code solver within the SCALE comprehensive modeling and simulation code. The diversity of data given in this report includes key actinides, stable fission products, and radioactive fission products. In general, when using the current ENDF/B-VII.0 nuclear data libraries in SCALE, the major actinides are predicted to within 5% of the measured values. Large improvements were seen for several of the curium isotopes when using improved cross section data found in evaluated nuclear data file ENDF/B-VII.0 as compared to ENDF/B-V-based results. The impact of the flux spectrum on the plutonium isotope concentrations as a function of burnup was also shown. The general accuracy noted for the actinide samples for reactor types with burnups greater than 5,000 MWd/MTU was not observed for the low-burnup Hanford B samples. More work is needed in understanding these large discrepancies. The stable neodymium and samarium isotopes were predicted to within a few percent of the measured values. Large improvements were seen in prediction for a few of the samarium isotopes when using the ENDF/B-VII.0 libraries compared to results obtained with ENDF/B-V libraries. Very accurate predictions were obtained for 133 Cs and 153 Eu. However, the predicted values for the stable ruthenium and rhodium isotopes varied as much as 10% of the measured values, and 109 Ag was consistently over-predicted by as much as 170%. In general, there is a larger uncertainty for modeling radioactive fission products when compared to either the actinides or the stable fission products in SNF. The relative C/E ratios ranged from a few percent for 137 Cs up to 60% and 100% for 106 Ru and 125 Sb, respectively. Limited or no radioactive fission products data exist in the current data sets for reactor types other than PWRs and BWRs. More work is needed in obtaining a greater diversity of radioactive fission product data. While performing this survey, issues leading to inconsistencies in nuclear fission yield data were discovered that specifically impacted the fission product noble gases. Emphasis was given to this legacy data, and corrective actions were taken as described in this report. After the fission yield data were corrected, the stable xenon and krypton fission products were predicted to within 5% of their measurements. However, preliminary results not explicitly given in this report indicate that the relative C/E ratio for the radioactive isotope 85 Kr varied as much as 10%. Due to the complex migration and the difficulty in measuring noble gases in the fuel, a more thorough investigation is needed to understand how accurately depletion codes can calculate these gas concentrations.
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We examine explosive nucleosynthesis of p-nuclei during a delayed neutrino-driven, aspherical supernova explosion aided by standing accretion shock instability, based on two-dimensional hydrodynamic simulations of the explosion of a 15M{sub {center_dot}} star. We find that p-nuclei are mainly produced through {gamma}-processes, and that the nuclei lighter than {sup 92}Mo are abundantly synthesized in slightly neutron-rich bubbles with electron fractions of Y{sub e}{<=}0.48. {sup 94}Mo, {sup 96}Ru, and {sup 98}Ru, are underproduced compared with the solar system, as in the spherical model.
The Q values of the neutrinoless double-electron capture transitions in {sup 96}Ru, {sup 162}Er, and {sup 168}Yb have been determined by Penning-trap mass-ratio measurements. Based on our new high-precision results for the Q values, neither of these transitions shows a resonant enhancement of the capture rate. At present, this excludes these nuclides from the list of suitable candidates in the search for neutrinoless double-electron capture.
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Beyond Fe, there is a class of 35 proton-rich nuclides, between {sup 74}Se and {sup 196}Hg, called p-nuclei. They are bypassed by the s and r neutron capture processes and are typically 10-1000 times less abundant than the s- and/or r-isotopes in the solar system. The bulk of p-isotopes is created in the 'gamma processes' by sequences of photodisintegrations and beta decays in explosive conditions in both core collapse supernovae (SNe II) and in Type Ia supernovae (SNe Ia). SNe II contribute to the production of p-nuclei through explosive neon and oxygen burning. However, the major problem in SN II ejecta is a general underproduction of the light p-nuclei for A < 120. We explore SNe Ia as p-process sites in the framework of a two-dimensional SN Ia delayed detonation model as well as pure deflagration models. The white dwarf precursor is assumed to have reached the Chandrasekhar mass in a binary system by mass accretion from a giant/main-sequence companion. We use enhanced s-seed distributions, with seeds directly obtained from a sequence of thermal pulse instabilities both in the asymptotic giant branch phase and in the accreted material. We apply the tracer-particle method to reconstruct the nucleosynthesis by the thermal histories of Lagrangian particles, passively advected in the hydrodynamic calculations. For each particle, we follow the explosive nucleosynthesis with a detailed nuclear reaction network for all isotopes up to {sup 209}Bi. We select tracers within the typical temperature range for p-process production, (1.5-3.7) x 10{sup 9} K, and analyze in detail their behavior, exploring the influence of different s-process distributions on the p-process nucleosynthesis. In addition, we discuss the sensitivity of p-process production to parameters of the explosion mechanism, taking into account the consequences on Fe and alpha elements. We find that SNe Ia can produce a large amount of p-nuclei, both the light p-nuclei below A = 120 and the heavy-p nuclei, at quite flat average production factors, tightly related to the s-process seed distribution. For the first time, we find a stellar source able to produce both light and heavy p-nuclei almost at the same level as {sup 56}Fe, including the debated neutron magic {sup 92,} {sup 94}Mo and {sup 96,} {sup 98}Ru. We also find that there is an important contribution from the p-process nucleosynthesis to the s-only nuclei {sup 80}Kr, {sup 86}Sr, to the neutron magic {sup 90}Zr, and to the neutron-rich {sup 96}Zr. Finally, we investigate the metallicity effect on p-process production in our models. Starting with different s-process seed distributions for two metallicities Z = 0.02 and Z = 0.001, running two-dimensional SN Ia models with different initial composition, we estimate that SNe Ia can contribute to at least 50% of the solar p-process composition. A more detailed analysis of the role of SNe Ia in Galactic chemical evolution of p-nuclei is in preparation.
The origin of ubiquitous nucleosynthetic isotope anomalies in meteorites may represent spatial and/or temporal heterogeneity in the sources that supplied material to the nascent solar nebula, or enhancement by chemical processing. For elements beyond the Fe peak, deficits in s-process isotopes have been reported in some (e.g., Mo, Ru, W) but not all refractory elements studied (e.g., Os) that, among the iron meteorites, are most pronounced in IVB iron meteorites. Palladium is a non-refractory element in the same mass region as Mo and Ru. In this study, we report the first precise Pd isotopic abundances from IVB irons to test the mechanisms proposed for the origin of isotope anomalies. First, this study determined the existence of a cosmogenic neutron dosimeter from the reaction {sup 103}Rh(n, β{sup −}){sup 104}Pd in the form of excess {sup 104}Pd, correlated with excess {sup 192}Pt, in IVB irons. Second, all IVB irons show a deficit of the s-process only isotope {sup 104}Pd (ε {sup 104}Pd = −0.48 ± 0.24), an excess of the r-only isotope {sup 110}Pd (ε{sup 110}Pd = +0.46 ± 0.12), and no resolvable anomaly in the p-process {sup 102}Pd (ε {sup 102}Pd = +1 ± 1). The magnitude of the Pd isotope anomaly is about half that predicted from a uniform depletion of the s-process yields from the correlated isotope anomalies of refractory Mo and Ru. The discrepancy is best understood as the result of nebular processing of the less refractory Pd, implying that all the observed nucleosynthetic anomalies in meteorites are likely to be isotopic relicts. The Mo–Ru–Pd isotope systematics do not support enhanced rates of the {sup 22}Ne(α,n){sup 25}Mg neutron source for the solar system s-process.
A common challenge for electrochemical ammonia synthesis in an aqueous phase is the consumption of Faradaic charge by the competing hydrogen evolution reaction (HER), which reduces the Faradaic efficiency for the desired conversion, i.e., the nitrate reduction reaction (NO 3 RR) to ammonium. This problem is particularly severe when a single-phase catalyst is operated at high current limits, thus a cocatalyst system that works synergistically for hydrogen acquisition and deoxygenation is needed to promote NO 3 RR over HER. For this study, we select a well-known HER catalyst Mo 2 C and investigate how metal doping can switch its kinetics from HER-dominated to NO 3 RR-dominated pathways. At 3.8 wt % Ru doping of Mo 2 C, a 75% single pass conversion of nitrate (0.1 M) to ammonium in a 16 cm 2 flow electrolyzer was achieved, corresponding to an ammonium yield rate of 9.07 mmol h –1 at a full cell voltage of 2 V. As confirmed by DFT calculations and kinetic isotope experiments, ruthenium dopants in the matrix serve as the sink point for adsorbed hydrogen during NO 3 RR to promote the cooperative deoxygenation of *NO 3 and *NO 2 on the Ru–Mo cocatalytic site. Our study suggests that optimizing hydrogen acquisition and deoxygenation reactions in cocatalytic systems is an effective strategy for electrochemical synthesis.
Photoneutron cross sections were extracted for isotopes of ruthenium and molybdenum on natural abundance targets via a reduced chi-squared analysis on excitation functions, or activation yields, as function of electron beam energy. Bremsstrahlung photons were produced via an electron linear accelerator and a tungsten radiator at the Idaho Accelerator Center. A total of 16 irradiations were performed with electron beam energies ranging from approximately 8 MeV to 23 MeV. Induced radioactivity was measured using a high purity germanium detector. The cross sections were extracted assuming a three parameter Lorentzian fit with a smooth truncated rise at reaction threshold.
We present the first measurements with a new collinear laser spectroscopy setup at the Argonne Tandem Linac Accelerator System, utilizing its unique capability to deliver neutron-rich refractory metal isotopes produced by the spontaneous fission of 252 Cf. We measured isotope shifts from optical spectra for nine radioactive ruthenium isotopes 106–114 Ru, reaching deep into the mid-shell region. The extracted charge radii are in excellent agreement with predictions from the Brussels-Skyrme-on-a-Grid models that account for the triaxial deformation of nuclear ground states. We show that triaxial deformation impacts charge radii in models that feature shell effects, in contrast to what could be concluded from a liquid drop analysis. This indicates that this exotic type of deformation should not be neglected in regions where it is known to occur, even if its presence cannot be unambiguously inferred through laser spectroscopy.
Cross section and S factor of the proton- and alpha-induced reactions have been studied for the Ruthenium and tin isotopes in the effective energy range, i.e. Gamow window. These reactions are important for developing the understanding for nucleosynthesis, particularly for the synthesis of p nuclei (p process). In this work, cross sections and S factor have been calculated through TALYS in Hauser–Feshbach formalism using nuclear densities calculated in relativistic mean field (RMF) formalism. Calculated results of cross sections, S factor and nuclear structure have been compared with existing theoretical as well as experimental results available and are found to be in good agreement.