Californium Rare Isotope Breeder Upgrade Research Articles

NuCARIBU : An upgrade for the CARIBU facility at the Argonne Tandem Linac Accelerator System

The Californium Rare Isotope Breeder Upgrade (CARIBU) facility is changing the mechanism for creating neutron-rich fission products. Spontaneous fission from a 252Cf source has provided beams to support the low energy and accelerated-beams ATLAS programs. 252Cf has a 2.65-year half-life, requiring the source to be replaced every three years to maintain high beam intensities. Fabricating an appropriately thin 252Cf source to efficiently release the fission products has been challenging. The solution to these problems is nuCARIBU, a new system that provides neutron-induced fission on actinide foils. The Best Cyclotron B6P System (6-MeV proton beam at 0.5mA) is chosen, utilizing a multi-cusp negative ion source extracting into a cyclotron, which uses carbon foils to strip the H- ions to protons. These protons are delivered to a 7Li target to produce neutrons. The fast neutrons are moderated to thermal energies to induce fission in an actinide foil, providing neutron-rich fission products. These subsystems are described in detail along with comparisons between the current CARIBU facility and the presented nuCARIBU facility.This work was supported by the U.S. Department of Energy, Office of Nuclear Physics, under Contract No. DE-AC02-06CH11357

New approach to precisely measure [formula omitted]-ray intensities for long-lived fission products, with results for the decay of 95Zr

For many fission products, the γ rays emitted following β decay provide an easily-detectable signature that can be used to identify their quantities and distributions in a sample. As a result, γ-ray spectroscopy is often exploited to study fission-product yields, provided sufficiently accurate information on the γ-ray intensity is available. However, in many cases, the uncertainties in the existing nuclear data are large enough that they compromise the precision achievable for modern experiments and applications. To address this need, we have developed a new experimental method that is well suited to precisely measure absolute γ-ray intensities in the β decay of long-lived fission products. The approach involves the production of a radiopure sample by implantation of a mass-separated ion beam from the CAlifornium Rare Isotope Breeder Upgrade (CARIBU) facility on a thin carbon foil. The emitted β-decay radiation is detected with a 4π gas proportional counter and a meticulously efficiency-calibrated high-purity germanium (HPGe) detector. As a first measurement to demonstrate the approach, we studied the absolute γ-ray intensities of the strongest transitions following the β decay of 95Zr and its decay-daughter 95Nb, and determined them to fractional precisions of better than 1–2%. In addition, with a larger sample of activity produced through neutron irradiation of an isotopically-enriched Zr foil, we performed a high-precision measurement of the relative γ-ray intensities following the decay of 95Zr with just the HPGe detector. The sample-production method at CARIBU and the coincidence detection approach demonstrated here can be applied to study fission products with half-lives longer than a day, which includes isotopes important not only for nuclear-energy and national-security applications, but also for medical-isotope research and environmental monitoring.

Spin-trap isomers in deformed, odd-odd nuclei in the light rare-earth region near N=98

Masses of neutron-rich, odd-odd Pm, Eu, and Tb nuclei near $N=98$ were measured using the Canadian Penning Trap mass spectrometer at the Californium Rare Isotope Breeder Upgrade (CARIBU) facility. High-resolution mass measurements yielded the discovery of spin-trap isomers at $N=97$ in $^{162}\mathrm{Tb}$, and in the $N=99$ isotones of $^{160}\mathrm{Pm}$ and $^{164}\mathrm{Tb}$. Furthermore, no evidence of long-lived isomers were observed at $N=95$ in $^{158}\mathrm{Eu}$, at $N=97$ in $^{158}\mathrm{Pm}$, nor at $N=101$ in $^{164}\mathrm{Eu}$ and $^{166}\mathrm{Tb}$. These experimental observations are compared to results from multiquasiparticle blocking calculations.

Improving the measurement sensitivity of the Canadian Penning Trap mass spectrometer through PI-ICR

For the past two decades the Canadian Penning Trap mass spectrometer (CPT) has been utilized to study various disciplines of nuclear physics through precision mass measurements. Since moving to the Californium Rare Isotope Breeder Upgrade (CARIBU) facility, the CPT experimental program has focused on neutron-rich nuclei whose masses may play an important role in the astrophysical r process. Through a recent upgrade of the detector system, the phase-imaging ion-cyclotron-resonance (PI-ICR) technique has been successfully implemented. This method offers several benefits which drastically improve the experimental sensitivity of the CPT to the most neutron-rich nuclei produced at CARIBU. Here we describe the PI-ICR procedure at the CPT, give an overview of the systematic sources of uncertainty in the system, and provide new mass results for 142I, 146La, and 163Gd which were made possible through this upgrade.

Masses and Beta-decay Studies of Neutron-rich Nuclei using the X-array and Gammasphere

Properties of neutron-rich nuclei in the A˜160 region are important for achieving a better understanding of the nuclear structure in this region where little is known owing to diffculties in the production of these nuclei at the present nuclear physics facilities. These properties are essential ingredients in the interpretation of the rareearth peak at A˜160 in the r process abundance distribution, since theoretical models are sensitive to nuclear structure input. Predicated on these ideas, we have initiated a new experimental program at Argonne National Laboratory. During the first experiment, beams from the Californium Rare Isotope Breeder Upgrade radioactive beam facility were used in conjunction with the SATURN decay station and the X-array. We focused initially on several odd-odd nuclei, where β decays of both the ground state and an excited isomer were investigated. Because of the spin difference, a variety of structures in the daughter nuclei were selectively populated and characterized based on their decay properties. Mass measurements using the Canadian Penning Trap aimed at establishing the excitation energy of the β-decaying isomers were also carried out. Evidence was found for a change in the single-particle structure, which in turn results in the formation of a sizable N=98 sub-shell gap at large deformation. Results from the first experimental campaign using the newly-commissioned β-decay station at Gammasphere are also presented.

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∼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 MonteCarlo technique. Our measured masses are consistent with the reverse-engineering predictions for a neutron star merger wind scenario.

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. 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.

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.

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 paper, we discuss the parameters of the EBIS and the charge breeding results in a pulsed injection mode with repetition rates up to 10 Hz.

Californium purification and electrodeposition

The staff at the Radiochemical Engineering Development Center, located at Oak Ridge National Laboratory, produced a 6.3 ± 0.4 GBq (1.7 ± 0.1 Ci) 252Cf source for the Californium Rare Isotope Breeder Upgrade (CARIBU) project at Argonne National Laboratory’s Argonne Tandem Linac Accelerator System. The source was produced by electrodeposition of a 252Cf sample onto a stainless steel substrate, which required material free from excess mass for efficient deposition. The resulting deposition was the largest reported 252Cf electrodeposition source ever produced. Several different chromatographic purification methods were investigated to determine which would be most effective for final purification of the feed material used for the CARIBU source. The separation of lanthanides from the Cf was of special concern. The separation, using 145Sm, 153Gd, and 249Cf as tracers, was investigated using BioRad AG 50X8 in α-hydroxyisobutyric acid, Eichrom LN resin in both HNO3 and HCl, and Eichrom TEVA resin in NH4SCN. The TEVA NH4SCN system was found to completely separate 145Sm and 153Gd from 249Cf and was adopted into the purification process used in purifying the 252Cf.

A Novel Approach to β-delayed Neutron Spectroscopy Using the Beta-decay Paul Trap

A new approach to β-delayed neutron spectroscopy has been demonstrated that circumvents the many limitations associated with neutron detection by instead inferring the decay branching ratios and energy spectra of the emitted neutrons by studying the nuclear recoil. Using the Beta-decay Paul Trap, fission-product ions were trapped and confined to within a 1-mm3 volume under vacuum using only electric fields. Results from recent measurements of 137I+ and plans for development of a dedicated ion trap for future experiments using the intense fission fragment beams from the Californium Rare Isotope Breeder Upgrade (CARIBU) facility at Argonne National Laboratory are summarized. The improved nuclear data that can be collected is needed in many fields of basic and applied science such as nuclear energy, nuclear astrophysics, and stockpile stewardship.

EBIS charge breeder for CARIBU

A high-efficiency charge breeder based on an Electron Beam Ion Source (EBIS) is being developed by the ANL Physics Division to increase the intensity and improve the purity of accelerated radioactive ion beams. A wide variety of low-energy neutron-rich ion beams are produced by the Californium Rare Isotope Breeder Upgrade (CARIBU) for the Argonne Tandem Linac Accelerator System (ATLAS). These beams will be charge-bred by an EBIS charge breeder to a charge-to-mass ratio (q/A) ≥ 1/7 and accelerated by ATLAS to energies of about 10 MeV/u. The assembly of the CARIBU EBIS charge breeder except the injection/extraction beam lines has been completed. This summer we started electron beam commissioning of the EBIS. The first results on electron beam extraction, transport from the electron gun to a high power electron collector are presented and discussed.

First Results from the CARIBU Facility: Mass Measurements on ther-Process Path

The Canadian Penning Trap mass spectrometer has made mass measurements of 33 neutron-rich nuclides provided by the new Californium Rare Isotope Breeder Upgrade facility at Argonne National Laboratory. The studied region includes the 132Sn double shell closure and ranges in Z from In to Cs, with Sn isotopes measured out to A=135, and the typical measurement precision is at the 100 ppb level or better. The region encompasses a possible major waiting point of the astrophysical r process, and the impact of the masses on the r process is shown through a series of simulations. These first-ever simulations with direct mass information on this waiting point show significant increases in waiting time at Sn and Sb in comparison with commonly used mass models, demonstrating the inadequacy of existing models for accurate r-process calculations.

Simulation and design of an electron beam ion source charge breeder for the californium rare isotope breeder upgrade

An electron beam ion source (EBIS) will be constructed and used to charge breed ions from the californium rare isotope breeder upgrade (CARIBU) for postacceleration into the Argonne tandem linear accelerator system (ATLAS). Simulations of the EBIS charge breeder performance and the related ion transport systems are reported. Propagation of the electron beam through the EBIS was verified, and the anticipated incident power density within the electron collector was identified. The full normalized acceptance of the charge breeder with a 2 A electron beam, $0.024\ensuremath{\pi}\text{ }\text{ }\mathrm{mm}\text{ }\mathrm{mrad}$ for nominal operating parameters, was determined by simulating ion injection into the EBIS. The optics of the ion transport lines were carefully optimized to achieve well-matched ion injection, to minimize emittance growth of the injected and extracted ion beams, and to enable adequate testing of the charge bred ions prior to installation in ATLAS.

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 (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 (143)Ba(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 (23)Na(7+) and 17.9% for (39)K(10+) were obtained injecting stable Na(+) and K(+) beams from a surface ionization source.

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(+) surface ionization ion source for external injection in pulsed mode. In these experiments we have achieved ∼70% injection∕extraction efficiency and breeding efficiency into the most abundant charge state of ∼17%.

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.

Studies of neutron-rich nuclei using the CPT mass spectrometer at CARIBU

The nucleosynthetic path of the astrophysical r-process and the resulting elemental abundances depend on neutron-separation energies which can be determined from the masses of the nuclei along the r-process reaction path. Due to the current lack of experimental data, mass models are often used. The mass values provided by the mass models are often too imprecise or disagree with each other. Therefore, direct high-precision mass measurements of neutron-rich nuclei are necessary to provide input parameters to the calculations and help refine the mass models. The Californium Rare Isotope Breeder Upgrade (CARIBU) facility of Argonne National Laboratory will provide experiments with beams of short-lived neutron-rich nuclei. The Canadian Penning Trap (CPT) mass spectrometer has been relocated to the CARIBU low-energy beam line to extend measurements of the neutron-rich nuclei into the mostly unexplored region along the r-process path. This will allow precise mass measurements (∼ 10 keV/c2) of more than a hundred very neutron-rich isotopes that have not previously been measured.

Measurements of charge state breeding efficiency at BNL test EBIS

Charge breeding of singly charged ions is required to efficiently accelerate rare isotope ion beams for nuclear and astrophysics experiments, and to enhance the accuracy of low-energy Penning trap-assisted spectroscopy. An efficient charge breeder for the Californium Rare Isotope Breeder Upgrade (CARIBU) to the ANL Tandem Linear Accelerator System (ATLAS) facility is being developed using the BNL Test Electron Beam Ion Source (Test EBIS) as a prototype. Parameters of the CARIBU EBIS charge breeder are similar to those of the BNL Test EBIS except the electron beam current will be adjustable in the range from 1 to 2 A. The electron beam current density in the CARIBU EBIS trap will be significantly higher than in existing operational charge state breeders based on the EBIS concept. The charge state breeding efficiency is expected to be about 25% for the isotope ions extracted from the CARIBU. For the success of our EBIS project, it is essential to demonstrate high breeding efficiency at the BNL Test EBIS tuned to the regime close to the parameters of the CARIBU EBIS at ANL. The breeding efficiency optimization and measurements have been successfully carried out using a Cs + surface ionization ion source for externally pulsed injection into the BNL Test EBIS. A Cs + ion beam with a total number of ions of 5×10 8 and optimized pulse length of 70 μs has been injected into the Test EBIS and charge-bred for 5.3 ms for two different electron beam currents – 1 and 1.5 A. In these experiments we have achieved 70% injection/extraction efficiency and breeding efficiency into the most abundant charge state ∼17%.

Expansion of the radioactive ion beam program at Argonne

The Argonne Tandem Linear Accelerator System (ATLAS) at Argonne National Laboratory (ANL) provides a wide range of stable ion beams and radioactive beams which have contributed to our understanding of nuclear structure and reactions. Until now, most radioactive ion beams at ATLAS were produced in flight using light-ion reactions such as (p, n), (d, n), (d, p), (d,3He), and (3He,n). Within the next few months, the radioactive ion beam program at ATLAS will acquire much extended, new capabilities with the commissioning of a new facility: the CAlifornium Rare Isotope Breeder Upgrade (CARIBU). CARIBU will supply ion beams of 252Cf fission fragments, which are thermalized in a gas catcher. The singly- and doubly-charged ions extracted from the gas catcher will be mass-separated and either delivered to a low-energy experimental area, or charge bred with a modified ECR source and subsequently reaccelerated by the ATLAS facility. Properties of hundreds of these neutron-rich nuclides will be investigated using ion traps, decay stations, the newly commissioned HELical Orbit Spectrometer (HELIOS), and other available experimental equipment such as Gammasphere and the FMA. HELIOS was constructed to take advantage of rare ion beams, such as those provided by CARIBU, through light-ion transfer reactions in inverse kinematics, and represents a new approach to the study of direct reactions in inverse kinematics which avoids kinematic broadening. Experiments are currently being conducted with HELIOS, and first results with the d(28Si,p) and d(12B,p) reactions have shown excellent energy resolution.