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At least 19 records

Development of electron beam ion source charge breeder for rare isotopes at Californium Rare Isotope Breeder Upgrade

Recently, the Californium Rare Isotope Breeder Upgrade (CARIBU) to the Argonne Tandem Linac Accelerator System (ATLAS) was commissioned and became available for production of rare isotopes. Currently, an electron cyclotron resonance ion source is used as a charge breeder for CARIBU beams. To further increase the intensity and improve the purity of neutron-rich ion beams accelerated by ATLAS, we are developing a high-efficiency charge breeder for CARIBU based on an electron beam ion source (EBIS). The CARIBU EBIS charge breeder will utilize the state-of-the-art EBIS technology recently developed at Brookhaven National Laboratory (BNL). The electron beam current density in the CARIBU EBIS trap will be significantly higher than that in existing operational charge-state breeders based on the EBIS concept. The design of the CARIBU EBIS charge breeder is nearly complete. Long-lead components of the EBIS such as a 6-T superconducting solenoid and an electron gun have been ordered with the delivery schedule in the fall of 2011. Measurements of expected breeding efficiency using the BNL Test EBIS have been performed using a Cs{sup +} surface ionization ion source for external injection in pulsed mode. In these experiments we have achieved {approx}70% injection/extraction efficiency and breeding efficiency into the most abundant charge state of {approx}17%.

43 PARTICLE ACCELERATORS↗

Fast and efficient charge breeding of the Californium rare isotope breeder upgrade electron beam ion source

The Electron Beam Ion Source (EBIS), developed to breed Californium Rare Isotope Breeder Upgrade (CARIBU) radioactive beams at Argonne Tandem Linac Accelerator System (ATLAS), is being tested off-line. A unique property of the EBIS is a combination of short breeding times, high repetition rates, and a large acceptance. Overall, we have implemented many innovative features during the design and construction of the CARIBU EBIS as compared to the existing EBIS breeders. The off-line charge breeding tests are being performed using a surface ionization source that produces singly charged cesium ions. The main goal of the off-line commissioning is to demonstrate stable operation of the EBIS at a 10 Hz repetition rate and a breeding efficiency into single charge state higher than 15%. These goals have been successfully achieved and exceeded. We have measured (20% ± 0.7%) breeding efficiency into the single charge state of 28+ cesium ions with the breeding time of 28 ms. In general, the current CARIBU EBIS operational parameters can provide charge breeding of any ions in the full mass range of periodic table with high efficiency, short breeding times, and sufficiently low charge-to-mass ratio, 1/6.3 for the heaviest masses, for further acceleration in ATLAS. In this study, we discuss the parameters of the EBIS and the charge breeding results in a pulsed injection mode with repetition rates up to 10 Hz.

43 PARTICLE ACCELERATORS↗

Design of the injection beamline for the Californium Rare Isotope Breeder Upgrade electron beam ion source charge breeder

The design of the ion injection line connecting the electron beam ion source (EBIS) charge breeder and the Californium Rare Isotope Breeder Upgrade radio frequency quadrupole cooler-buncher at the Argonne Tandem Linear Accelerator System was investigated with particle tracking simulations. The injection line was configured to accommodate several differential pumping sections, individual optical components were optimized to minimize emittance growth, and the ion beam parameters were matched with the EBIS electron beam acceptance to minimize losses upon injection.

43 PARTICLE ACCELERATORS↗

Electrodeposition method development for Californium Rare Isotope Breeder Upgrade (CARIBU) Source

Electrodeposition is one of the most widely utilized techniques for thin-film production with high yields. Although it is used extensively, this technique still presents several issues limiting its usefulness, including excess thickness and frequent cracking of deposited films. Efforts to improve thin-film production recently undertaken at Oak Ridge Laboratory by the authors have included studying operating conditions and applied electrolytes. Samarium was used as a surrogate material for californium, and yield was compared with different deposition condition. The final procedure from the optimized condition will be applied during production of the californium-252 source for the Californium Rare Isotope Breeder Upgrade (CARIBU) project, and the fission fragment will be analyzed.

07 ISOTOPE AND RADIATION SOURCES↗

MANTA. An Integral Reactor Physics Experiment to Infer the Neutron Capture Cross Sections of Actinides and Fission Products in Fast and Epithermal Spectra

Neutron cross-sections characterize the way neutrons interact with matter. They are essential to most nuclear engineering projects and, even though theoretical progress has been made as far as the predictability of neutron cross-section models, measurements are still indispensable to meet tight design requirements for reduced uncertainties. Within the field of fission reactor technology, one can identify the following specializations that rely on the availability of accurate neutron cross-sections: (1) fission reactor design, (2) nuclear fuel cycles, (3) nuclear safety, (4) nuclear safeguards, (5) reactor monitoring and neutron fluence determination and (6) waste disposal and transmutation. In particular, the assessment of advanced fuel cycles requires an extensive knowledge of transuranics cross sections. Plutonium isotopes, but also americium, curium and up to californium isotope data are required with a small uncertainty in order to optimize significant features of the fuel cycle that have an impact on feasibility studies (e.g. neutron doses at fuel fabrication, decay heat in a repository, etc.). Different techniques are available to determine neutron cross sections experimentally, with the common denominator that a source of neutrons is necessary. It can either come from an accelerator that produces neutrons as a result of interactions between charged particles and a target, or it can come from a nuclear reactor. When the measurements are performed with an accelerator, they are referred to as differential since the analysis of the data provides the cross-sections for different discrete energies, i.e. σ(E i ), and for the diffusion cross sections for different discrete angles. Another approach is to irradiate a very pure sample in a test reactor such as the Advanced Test Reactor (ATR) at INL and, after a given time, determine the amount of the different transmutation products. The precise characterization of the nuclide densities before and after neutron irradiation allows to infer energy-integrated neutron cross sections, i.e. ∫₀ ∞ σ(E)φ(E)dE, where φ(E) is the neutron flux “seen” by the sample. This approach, which is usually defined and led by reactor physicists, is referred to as integral and is the object of this report. These two sources of information, i.e. differential and integral, are complementary and are used by the nuclear physicists in charge of producing the evaluated nuclear data files used by the nuclear community (ENDF, JEFF…). The generation of accurate nuclear data files requires an iterative process involving reactor physicists and nuclear data evaluators. This experimental program has been funded by the ATR National Scientific User Facility (ATR-NSUF) and by the DOE Office of Science in the framework of the Recovery Act. It has been given the name MANTRA for Measurement of Actinides Neutron TRAnsmutation.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Californium Electrodepositions at Oak Ridge National Laboratory

Electrodepositions of californium isotopes were successfully performed at Oak Ridge National Laboratory (ORNL) during the past year involving two different types of deposition solutions, ammonium acetate (NH 4 C 2 H 3 O 2 ) and isobutanol ((CH 3 ) 2 CHCH 2 OH). A californium product that was decay enriched in 251 Cf was recovered for use in super-heavy element (SHE) research. This neutron-rich isotope, 251 Cf, provides target material for SHE research for the potential discovery of heavier isotopes of Z=118. The californium material was recovered from aged 252 Cf neutron sources in storage at ORNL. These sources have decayed for over 30 years, thus providing material with a very high 251 Cf-to- 252 Cf ratio. After the source capsules were opened, the californium was purified and then electrodeposited using the isobutanol method onto thin titanium foils for use in an accelerator at the Joint Institute for Nuclear Research in Dubna, Russia. Another deposition method, ammonium acetate, was used to produce a deposition containing 1.7 0.1 Ci of 252 Cf onto a stainless steel substrate. This was the largest single electrodeposition of 252 Cf ever prepared. The 252 Cf material was initially purified using traditional ion exchange media, such as AG50-AHIB and AG50-HCl, and further purified using a TEVA-NH 4 SCN system to remove any lanthanides, resulting in the recovery of 3.6 0.1 mg of purified 252 Cf. The ammonium acetate deposition was run with a current of 1.0 amp, resulting in a 91.5% deposition yield. Purification and handling of the highly radioactive californium material created additional challenges in the production of these sources.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Moderator design studies for a new neutron reference source based on the $\mathrm{D}$–$\mathrm{T}$ fusion reaction

The radioactive isotope Californium-252 ( 252 Cf) is relied upon internationally as a neutron calibration source for ionizing radiation dosimetry because of its high specific activity. The source may be placed within a heavy-water (D 2 O) moderating sphere to produce a softened spectrum representative of neutron fields common to commercial nuclear power plant environments, among others. Due to termination of the U.S. Department of Energy loan/lease program in 2012, the expense of obtaining 252 Cf sources has undergone a significant increase, rendering high output sources largely unattainable. On the other hand, the use of neutron generators in research and industry applications has increased dramatically in recent years. Neutron generators based on deuterium-tritium (D-T) fusion reaction provide high neutron fluence rates and, therefore, could possibly be used as a replacement for 252 Cf. To be viable, the 14.6 MeV D-T output spectrum must be significantly moderated to approximate common workplace environments. Here this paper presents the results of an effort to select appropriate moderating materials and design a configuration to reshape the primary neutron field toward a spectrum approaching that from a nuclear power plant workplace. A series of Monte-Carlo (MCNP) simulations of single layer high- and low-Z materials are used to identify initial candidate moderators. Candidates are refined through a similar series of simulations involving combinations of 2 to 5 different materials. The simulated energy distribution using these candidate moderators are rated in comparison to a target spectrum. Other properties, such as fluence preservation and/or enhancement, prompt gamma production and other characteristics are also considered.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Guide for Employing High-Resolution Gamma Spectroscopy for 252Cf Source Age and Isotopic Composition

Californium-252 is commonly used as a calibration source for neutron coincidence and neutron multiplicity counting in nuclear safeguards. Accurate knowledge of the neutron emission rate, age, and isotopics of the source (i.e., “source term”) are important for ensuring the best possible accuracies in item assay results. Californium-252 sources are not usually measured using gamma spectrometry, because of the assumption that their gamma-ray spectra appear to provide little information. However, gamma-ray signatures produced from 252Cf spontaneous fission products and odd-numbered Cf isotopes can be useful in determining source age and Cf isotopic composition. We demonstrate the utility of high-resolution gamma spectrometry in determining the age and isotopics of Cf neutron sources. In this work, five 252Cf sources were measured using a high-purity germanium detector. The neutron flux was small enough that radiation damage from prolonged neutron exposure was not substantial. Spectra were collected in 2-hour increments for 42–48 hours for quality control. The 2-hour spectra were added together to create a single spectrum for each source, and peak analyses were performed. Source ages were determined using a method that involved experimentally measuring the ratio of the gamma-ray emission rate of the 661.657 keV from 137Cs relative to a short-lived fission product and exploiting the dependence of this ratio on the source age. Source age was solved for using emission rates from four different gamma lines from four short-lived spontaneous fission products. Analysis results from all four fission products returned statistically similar source ages, but two had uncertainties greater than 25% because of high spontaneous fission product yield uncertainties as nominally high as 63%. Choosing short-lived fission products with small yield uncertainties is most important for accurately calculating source age. Additionally, the calculated ages did not always match the time since 248Cm separation well, which is often assumed to be the source age on the technical data sheet provided by the manufacturer. Activity ratios of 249Cf to 251Cf, the only Cf gamma emitters present in a 252Cf source, also did not match between experimental data and data on the technical data sheet provided by the vendor. It is thus recommended that newly purchased Cf sources be examined using gamma spectrometry to determine the source age and confirm isotopic composition of a 252Cf calibration source.

Watson, Mara M.↗

Investigating the effects of precise mass measurements of Ru and Pd isotopes on machine learning mass modeling

Atomic masses are a foundational quantity in our understanding of nuclear structure, astrophysics, and fundamental symmetries. The longstanding goal of creating a predictive global model for the binding energy of a nucleus remains a significant challenge, however, and prompts the need for precise measurements of atomic masses to serve as anchor points for model developments. We present precise mass measurements of neutron-rich Ru and Pd isotopes performed at the Californium Rare Isotope Breeder Upgrade facility at Argonne National Laboratory using the Canadian Penning Trap mass spectrometer. The masses of 108 Ru, 110 Ru, and 116 Pd were measured to a relative mass precision $\delta$⁢$m/m$ ≈ 10 -8 via the phase-imaging ion-cyclotron-resonance technique, and represent an improvement of approximately an order of magnitude over previous measurements. Further, these mass data were used in conjunction with the physically interpretable machine learning (PIML) model, which uses a mixture density neural network to model mass excesses via a mixture of Gaussian distributions. The effects of our new mass data on a Bayesian-updating of a PIML model are presented.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Precision Mass Measurements of Neutron-Rich Neodymium and Samarium Isotopes and Their Role in Understanding Rare-Earth Peak Formation

The Canadian Penning Trap mass spectrometer at the Californium Rare Isotope Breeder Upgrade (CARIBU) facility was used to measure the masses of eight neutron-rich isotopes of Nd and Sm. These measurements are the first to push into the region of nuclear masses relevant to the formation of the rare-earth abundance peak at A similar to 165 by the rapid neutron-capture process. We compare our results with theoretical predictions obtained from "reverse engineering" the mass surface that best reproduces the observed solar abundances in this region through a Markov chain Monte Carlo technique. Our measured masses are consistent with the reverse-engineering predictions for a neutron star merger wind scenario.

Orford, R.↗

Off-line commissioning of EBIS and plans for its integration into ATLAS and CARIBU

An Electron Beam Ion Source Charge Breeder (EBIS-CB) has been developed at Argonne to breed radioactive beams from the CAlifornium Rare Isotope Breeder Upgrade (CARIBU) facility at Argonne Tandem Linac Accelerator System (ATLAS). The EBIS-CB will replace the existing ECR charge breeder to increase the intensity and significantly improve the purity of reaccelerated radioactive ion beams. The CARIBU EBIS-CB has been successfully commissioned offline with an external singly charged cesium ion source. The performance of the EBIS fully meets the specifications to breed rare isotope beams delivered from CARIBU. The EBIS is being relocated and integrated into ATLAS and CARIBU. A long electrostatic beam transport system including two 180° bends in the vertical plane has been designed. The commissioning of the EBIS and the beam transport system in their permanent location will start at the end of this year.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Masses and β-Decay Spectroscopy of Neutron-Rich Odd-Odd 160,162 Eu Nuclei: Evidence for a Subshell Gap with Large Deformation at N = 98

The structure of deformed neutron-rich nuclei in the rare-earth region is of significant interest for both the astrophysics and nuclear structure fields. At present, a complete explanation for the observed peak in the elemental abundances at A ~ 160 eludes astrophysicists, and models depend on accurate quantities, such as masses, lifetimes, and branching ratios of deformed neutron-rich nuclei in this region. Unusual nuclear structure effects are also observed, such as the unexpectedly low energies of the first 2 + levels in some even-even nuclei at N = 98. In order to address these issues, mass and β-decay spectroscopy measurements of the 160 Eu 97 and 162 Eu 99 nuclei were performed at the Californium Rare Isotope Breeder Upgrade radioactive beam facility at Argonne National Laboratory. Here, evidence for a gap in the single-particle neutron energies at N = 98 and for large deformation (β 2 ~ 0.3) is discussed in relation to the unusual phenomena observed at this neutron number.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Design of the low energy beam transport line between CARIBU and the EBIS charge breeder

An Electron Beam Ion Source Charge Breeder (EBIS-CB) has been developed to breed radioactive beams from the CAlifornium Rare Isotope Breeder Upgrade (CARIBU) facility at ATLAS. The EBIS-CB will replace the existing ECR charge breeder to increase the intensity and improve the purity of reaccelerated radioactive ion beams. The EBIS-CB is in the final stage of off-line commissioning. Currently, we are developing a low energy beam transport (LEBT) system to transfer CARIBU beams to the EBIS-CB. As was originally planned, an RFQ cooler-buncher will precede the EBIS-CB. Recently, it was decided to include a multi-reflection time-of-flight (MR-TOF) mass-spectrometer following the RFQ. MR-TOF is a relatively new technology used to purify beams with a mass-resolving power up to 3×10{sup 5} as was demonstrated in experiments at CERN/ISOLDE. Very high purity singly-charged radioactive ion beams will be injected into the EBIS for charge breeding and due to its inherent properties, the EBIS-CB will maintain the purity of the charge bred beams. Possible contamination of residual gas ions will be greatly suppressed by achieving ultra-high vacuum in the EBIS trap. This paper will present and discuss the design of the LEBT and the overall integration of the EBIS-CB into ATLAS.

43 PARTICLE ACCELERATORS↗

Improved charge breeding efficiency of light ions with an electron cyclotron resonance ion source

The Californium Rare Isotope Breeder Upgrade is a new radioactive beam facility for the Argonne Tandem Linac Accelerator System (ATLAS). The facility utilizes a {sup 252}Cf fission source coupled with an electron cyclotron resonance ion source to provide radioactive beam species for the ATLAS experimental program. The californium fission fragment distribution provides nuclei in the mid-mass range which are difficult to extract from production targets using the isotope separation on line technique and are not well populated by low-energy fission of uranium. To date the charge breeding program has focused on optimizing these mid-mass beams, achieving high charge breeding efficiencies of both gaseous and solid species including 14.7% for the radioactive species {sup 143}Ba{sup 27+}. In an effort to better understand the charge breeding mechanism, we have recently focused on the low-mass species sodium and potassium which up to present have been difficult to charge breed efficiently. Unprecedented charge breeding efficiencies of 10.1% for {sup 23}Na{sup 7+} and 17.9% for {sup 39}K{sup 10+} were obtained injecting stable Na{sup +} and K{sup +} beams from a surface ionization source.

43 PARTICLE ACCELERATORS↗

Assembly and commissioning of a new SRF cryomodule for the ATLAS intensity upgrade

The Argonne National Laboratory Physics Division is in the final stages of a major upgrade to the Argonne Tandem Linear Accelerator System national user facility, referred to as the intensity upgrade. The intensity upgrade project will substantially increase beam currents for experimenters working with the existing ATLAS stable and in-flight rare isotope beams and for the neutron-rich beams from the Californium Rare Isotope Breeder Upgrade. This project includes the replacement of three existing cryomodules, containing 18 superconducting accelerator cavities and 9 superconducting solenoids, with a single cryomodule with seven SC 72.75 MHz accelerator cavities optimized for ion velocities of 7.7% the speed of light and 4 SC solenoids all operating at 4.5 K. This presentation will report: how we minimized the heat load into the 4 K and 80 K coolant streams feeding the cryomodule, a comparison of the calculated and measured static heat loads at 80 K and the mechanical design of the vacuum vessel.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Californium-252 production at the High Flux Isotope Reactor - II: Comparison between the highly enriched uranium and a proposed low-enriched uranium core

This is the second paper on a 252 Cf production study performed in support of efforts to convert the High Flux Isotope Reactor (HFIR) from highly enriched uranium (HEU) to low-enriched uranium (LEU) fuel. The first paper primarily focuses on validating computational tools and nuclear data. This companion paper evaluates another critical aspect: the 252 Cf production capability with a proposed LEU core. HFIR must maintain its world-class performance and missions following conversion and because 252 Cf is a vital, multipurpose neutron-emitting radioisotope, the ability to efficiently produce 252 Cf must be preserved. In this study, the HFIRCON transport and depletion tool, several nuclear data libraries, and Campaign 78 data were used to compute 252 Cf production, sensitivity, and safety metrics. Further, results indicate the 252 Cf production and production rates are slightly higher with a 95MW th LEU core compared with those obtained with the 85MW th HEU core. Additionally, the target peak fission rate densities, discharge cumulative fission densities, and heat deposition rates with the LEU core are within a few percent of those calculated with the HEU core. The findings suggest HFIR’s 252 Cf production capability can be effectively maintained with an LEU core without adversely affecting the safety metrics.

07 ISOTOPE AND RADIATION SOURCES↗

Californium-252 production at the High Flux Isotope Reactor - I: Validation study using campaign data

This paper presents a series of 252 Cf production validation and code-to-code comparison studies performed based on data from the production campaigns at the High Flux Isotope Reactor (HFIR). These studies support efforts to convert HFIR from using highly enriched uranium (HEU) fuel to low-enriched uranium (LEU) fuel. HFIR must maintain its world-class performance and missions following this conversion, and because 252 Cf is a vital neutron-emitting radioisotope used for a variety of high-impact applications (e.g., reactor startup, cancer treatment), the ability to efficiently produce 252 Cf must be preserved. In this work, the HFIRCON, Shift, ORIGEN, and TCOMP codes were deployed, and several sets of data libraries were investigated to better understand the calculation codes and the data biases. As-loaded target composition data, as-run irradiation history data, and post-irradiation measurements from recent multi-cycle irradiation campaigns of the HEU core were used to validate and determine methodology biases. Further, the findings demonstrated a good agreement, with results falling within 3 standard deviations of measurements. This paper lays the ground work for the second paper, which evaluates and compares 252 Cf production and safety metrics with the HEU core and a proposed LEU core.

07 ISOTOPE AND RADIATION SOURCES↗