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Considerations on the design of a rare isotope beam facility based on superconducting heavy ion linacs

To establish an accelerator facility based on superconducting linear accelerator (linac) for nuclear and applied sciences in Korea, the rare isotope science project started in December 2011 under the auspices of the Institute for Basic Science (IBS). The layout of the facility has been mostly frozen since 2013 and civil construction began in 2016. On the other hand, an alternative linac design option was recently investigated in collaboration with the linac development group of Argonne National Lab in search of a further optimized configuration. A new linac lattice was developed and evaluated against realistic machine errors using TRACK. The beam optics simulations and error analysis then proved the soundness of this alternative design. In addition, beam optics of the injector was studied for simultaneous acceleration of both stable and rare isotope beams with the use of an electron beam ion source (EBIS). Additionally considered are alternative options of high-power cyclotrons as ISOL driver in order to enhance the capability of rare isotope beam production and fully exploit the superconducting linac facility built at high cost.

07 ISOTOPE AND RADIATION SOURCES↗

NACS 2022 FRIB Investment Strategy

The Facility for Rare Isotope Beams (FRIB) that will begin operations later this year will vastly increase the number of unstable isotopes available for experiments that, together with new theoretical developments will expand our understanding of nuclear structure and nuclear reactions that produce the elements of the periodic table and power the cosmos. The knowledge and understanding gained from FRIB will benefit a variety of applications including stockpile science, nuclear forensics, nonproliferation, nuclear energy, and nuclear medicine. LLNL is actively involved in a variety of basic and applied science activities related to FRIB. These activities are listed below and documented in the following sections: 1. FRIB Decay Station, 2. Isotope Harvesting, 3. Direct Reactions, 4. Surrogate Reactions, 5. Nuclear Structure and Collectivity, 6. Nuclear Fission, and 7. Nuclear Theory.

07 ISOTOPE AND RADIATION SOURCES↗

Physics Division Strategic Plan Fiscal Years 2020-2024

The vision of the Physics Division (PHY) at Argonne National Laboratory is to continue enhancing its role as a world-leading institution in basic nuclear physics research and its applications. Key to this vision is for PHY to continue to safely and effectively operate and evolve the capabilities of the Argonne Tandem Linac Accelerator System (ATLAS) facility to best serve its users. ATLAS is the Department of Energy (DOE) accelerator facility for low-energy nuclear physics research. The research carried out by PHY covers many themes in contemporary science but can be distilled into five areas of focus. These themes are interconnected, with continuously evolving synergies between the various groups and facilities in PHY and the broader Laboratory. This five-year strategic plan serves to illustrate our current capabilities and new directions related to these five areas of focus (ATLAS also develops an independent strategic plan): Accelerator research and design. The goal of this theme is to design, fabricate, test, and implement novel accelerator systems, with a focus on high-intensity ion and electron systems. These R&D activities have led to enhancements in the ATLAS accelerator system. Among others, the division’s accelerator systems are in use or planned for use at Fermilab, the Advanced Photon Source, and in a broad variety of applications at the Facility for Rare Isotope Beams (FRIB). Atom trapping and fundamental symmetries. The goal of this theme is to explore and exploit the uses of advanced laser cooling and trapping techniques to manipulate atoms. There are three main areas of focus. First is in the application of the atom trap trace analysis (ATTA) technique for age determination of groundwater and ice by using radio-krypton dating. The next two trapping-based programs involve tests of fundamental symmetries in nature: the cooling and trapping of radium-225 with the aim of determining limits on an observation of its electric dipole moment and precision measurements of the beta decay properties of helium-6 to set limits on the tensor coupling constant. This is complemented by measurements of similar properties in lithium-8 and boron-8. Nuclear astrophysics. The goal of this theme is to enhance our understanding of how elements are created in the universe via explosive nucleosynthesis and how stars evolve. To meet the challenges of this theme, many of the capabilities of ATLAS are being enhanced, including the development of new beams through a new in-flight separator (RAISOR) and the anticipated neutron-generator upgrade of the Californium Rare Isotope Breeder Upgrade facility (nuCARIBU). These are coupled to state-of-the-art instruments such as the Canadian Penning Trap, Helical Orbit Spectrometer, Gammasphere, GRETINA, Multi-Sampling Ionization Chamber, the Fragment Mass Analyzer, and Argonne Gas-filled Fragment Analyzer, and a new low-background experimental area for decay studies. Nuclear structure. The goal of this theme is to understand the structure of nuclei, both stable and radioactive, in terms of single-particle properties, their shapes, and the dynamics governing reactions between them. These include questions such as what are the limits of nuclear stability and what are the properties of super heavy nuclei. As with the nuclear astrophysics theme, the capabilities of ATLAS, guided by the ATLAS user community, are continuously being enhanced to this end. The Division has strategic initiatives to play a leading role in the development of instrumentation and research programs at the FRIB. Quantum chromodynamics (QCD) and hadron physics. The goal of this theme is to lead major research programs focused on revealing the quark and gluon structure of protons, neutrons, nuclei, and short-lived mesons and baryons. These involve major programs at Jefferson Lab, Fermilab, and smaller facilities. They are complemented by theoretical endeavors centered on the question of how hadrons and their properties emerge from QCD. Out of these activities arise strategic initiatives to play a major role in the forthcoming Electron-Ion Collider (EIC).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Commissioning of an MPGD-based Drift Chamber for Heavy-ion Tracking in FRIB's Sweeper magnet system

A newly developed drift chamber equipped with an innovative hybrid Micro-Pattern Gaseous Detector based readout was commissioned at FRIB. The detector consists of a Multi-layer Thick Gas Electron Multiplier (M-THGEM) mounted over a high-granularity, position-sensitive readout board. Denoted as the Micro-Pattern Drift Chamber (MPDC), the new device is used to provide tracking capability as part of the detectors of the Sweeper magnet system for neutron-invariant-mass spectrometry at the Facility for Rare Isotope Beams (FRIB). The localization of impinging ions in a 30 × 30 cm 2 drift area is derived by processing the charge-avalanche distribution induced on the segmented readout board. The signals induced on the readout pads are processed by a compact, multi-channel Data Acquisition System (DAQ) based on the Scalable Readout System (SRS). To facilitate synchronization with other detector systems of the Sweeper magnet system, the SRS has been configured to accept an external trigger.

Gaseous detectors↗

Crossing N = 28 Toward the Neutron Drip Line: First Measurement of Half-Lives at FRIB

Here, new half-lives for exotic isotopes approaching the neutron drip-line in the vicinity of N~28 for Z=12–15 were measured at the Facility for Rare Isotope Beams (FRIB) with the FRIB decay station initiator. The first experimental results are compared to the latest quasiparticle random phase approximation and shell-model calculations. Overall, the measured half-lives are consistent with the available theoretical descriptions and suggest a well-developed region of deformation below 48 Ca in the N=28 isotones. The erosion of the Z=14 subshell closure in Si is experimentally confirmed at N=28, and a reduction in the 38 Mg half-life is observed as compared with its isotopic neighbors, which does not seem to be predicted well based on the decay energy and deformation trends. This highlights the need for both additional data in this very exotic region, and for more advanced theoretical efforts.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Commissioning of the Advanced Rare Isotope Separator ARIS at FRIB

The Facility for Rare Isotope Beams (FRIB) at Michigan State University (MSU) consists of a newly constructed linear accelerator and fragment separator that are designed for enhanced production rates of rare isotopes for use in research and other societal applications. Recent activities through to August 2022 took place to commission the Advanced Rare Isotope Separator (ARIS) and carry out the first experiments. This followed commissioning of the newly constructed linac that is designed to provide orders of magnitude higher beam power than the previously coupled cyclotrons. This required that more advanced target, beam dump, and collimation systems of the new separator be designed and constructed to sustain unprecedented conditions by heavy ion beams. Commissioning with ~1 kW beams began recently and results from activities that began in late 2021 are reported here. Comparisons between the previous and current facilities are provided.

43 PARTICLE ACCELERATORS↗

The nu-process

As the core of a massive star collapses to form a neutron star, the flux of neutrinos in the overlying shells of heavy elements becomes so great that, despite the small cross section, substantial nuclear transmutation is induced. Neutrinos excite heavy elements and even helium to particle unbound levels. The evaporation of a single neutron or proton, and the back reaction of these nucleons on other species present, significantly alters the outcome of traditional nucleosynthesis calculations leading to a new process: nu-nucleosynthesis. Modifications to traditional hydrostatic and explosive varieties of helium, carbon, neon, oxygen, and silicon burning are considered. The results show that a large number of rare isotopes, including many of the odd-Z nuclei from boron through copper, owe much of their present abundance in nature to this process.

Woosley, S. E.↗

SPIRIT - A high resolution cosmic ray isotope spectrometer for Spacelab

An instrument to measure the isotopic abundances of cosmic ray nuclei with Z in the range 20-30 and A in the range 40-70 has been conceived. The instrument, named SPIRIT (Superconducting Passive Iron Isotope Telescope), will have the mass resolution (sigma less than 0.15 amu) and collecting power (151 sq m ster h for a 10 day flight) to detect and convincingly resolve isotopes as rare as 0.5% of the total abundance of each element. Both range and magnetic rigidity are measured by following tracks through an array of sheets of CR-39, a sensitive new track-recording plastic, which had been kept in fixed position at uniform temperature within the uniform field region of a large superconducting magnet.

Tarle, G.↗

A radioisotope - enabled reactive transport model for deep vadose zone carbon

In mountainous regions, which constitute the principle source of recharge to major rivers and regional aquifers, infiltration occurs through fractured, partially saturated, weathered bedrock that acts as a boundary layer between saturated aquifers and surface soil. Commonly this deep vadose zone (DVZ) is many meters thick, and yet its role in regulating the generation, retention and mobility of reactive solutes, including nutrients, contaminants and weathering products, is largely unknown. In particular, many of the key reactions that drive the formation of the weathered DVZ and the quality of water moving through it are redox processes, regulated by the availability of organic carbon and oxygen below the soil layer. The role of the DVZ is thus also poorly constrained in the context of carbon stocks and mobility, particularly in lithologies that are naturally high in organic carbon, such as shales. The overarching hypothesis of this study is that upland regions developed in geologic settings with abundant petrogenic carbon store and actively cycle carbon in the weathered DVZ below the soil and above the water table at rates that are significant and currently unconstrained. In order to quantify this cycling, the current study combines novel instrumentation techniques allowing new direct sampling of DVZ systems with advanced numerical reactive transport simulations of carbon transport and transformation. Critically, these simulations will explicitly treat the three isotopes of carbon (the abundant 12C, the stable rare 13C and the radioactive 14C) in a unified framework, thus clearly parsing between the contributions of modern surface derived carbon and lithologic carbon sources in integrated measurements of fluid and gas phase fluxes. This novel model capability will be applied to test the role of DVZ carbon cycling as a regulator of water quality and geological weathering in two complementary field sites both located in organic carbon rich shale lithologies. The first is the Eel River Critical Zone Observatory (ERCZO) in Mendocino County, California, and the second is the Lawrence Berkeley National Laboratory Watershed Function Scientific Focus Area (SFA) in the East River watershed, near Crested Butte, Colorado. At the ERCZO, a novel vadose zone monitoring system has been installed in a 20 m thick, partially saturated, weathered shale hillslope, and preliminary data already indicate substantial CO2 flux generated many meters below the soil surface. At the SFA field site, an instrumented hillslope transect indicates a more complex multi-dimensional fluid and solute transport regime, which will serve as a key test of the calibrated models. Collectively, this project will advance understanding of the cycling of carbon belowground and in relation to transport pathways across the poorly constrained DVZ characteristic of primary water recharge areas. The key product of this work will be enhanced isotope simulation capabilities that are robust and publicly available for application across a broad diversity of systems.

58 GEOSCIENCES↗

Development of a High Resolution-High Sensitivity Ion Microprobe Facility for Cosmochemical Applications

NASA NAGW-4112 has supported development of the CAMECA ims 1270 ion microprobe at UCLA for applications in cosmochemistry. The instrument has been brought to an operational status and techniques developed for accurate, precise microbeam analysis of oxygen isotope ratios in polished thin-sections. We made the first oxygen isotopic (delta(18)O and delta(17)O) measurements of rare mafic silicates in the most chemically primitive meteorites, the a chondrites (Leshin et al., 1997). The results have implications for both high temperature processing in the nebula and low-T aqueous alteration on the CI asteroid. We have performed measurements of oxygen isotopic compositions of magnetite and co-existing olivine from carbonaceous (Choi et al., 1997) and unequilibrated ordinary chondrites (Choi et al., in press). This work has identified a significant new oxygen isotope reservoir in the early solar system: water characterized by a very high Delta(17)) value of approx. 5 % per thousand. We have determined the spatial distributions of oxygen isotopic anomalies in all major mineral phases of a type B CAI from Allende. We have also studied an unusual fractionated CAI from Leoville and made the first oxygen isotopic measurements in rare CAIs from ordinary chondrites.

McKeegan, Kevin D.↗

Opportunities for isomer studies for astrophysics at FRIB

The role of nuclear isomers in astrophysical nucleosynthesis is gaining increased attention, as reactions on ground and isomeric states are both potentially important for determining the reaction rates and flow within the reaction network. A particular case is the odd-odd N=Z nuclides in the sd -shell, which play an important role in breakout from the CNO cycle in nova nucleosynthesis, affecting reaction flow, the nucleosynthesis end-point, and final abundances, impacting potential astronomical observables. Because many of these nuclides have low-lying isomers, it is important to constrain reactions on both ground and isomeric states. Developments in radioactive-beam facilities are opening such opportunities, via direct and indirect techniques. The first measurement using a new technique for manipulating ground/isomer content in reaccelerated beams without affecting ion optics, has been employed to study 38 K, which will be applicable to measurements on 34 Cl and others at the nascent Facility for Rare Isotope Beams.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Fission-product decay studies with the FRIB Decay Station

The Facility for Rare Isotopes Beams (FRIB) will be the flagship facility in low-energy nuclear physics when it comes online in 2022. This U.S. Department of Energy Office of Science user facility will open up a multitude of new opportunities to study exotic nuclei and will lead to new discoveries in nuclear structure, nuclear astrophysics, fundamental symmetries, and isotopes of importance to nuclear applications. The b-decay properties of neutron-rich isotopes will be measured with the FRIB Decay Station, a sophisticated state-of-the-art modular multi-detector system envisioned to perform b, g, n, and charged-particle spectroscopy. In this feasibility study, we use nuclear decay data collected with the FRIB Decay Station precursor, the Beta-Counting Station, currently used at Michigan State University with a radioactive beam produced at the National Superconducting Cyclotron Laboratory to identify the FRIB Decay Station capabilities for future measurements of neutron-rich exotic nuclei at FRIB to help provide a path forward for future measurements of interest to the lab’s mission.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Identification of an interstellar oxide grain from the Murchison meteorite by ion imaging

We report here the first use of a new ion-imaging system to locate a rare interstellar aluminum oxide grain in a Murchison acid residue. While several types of carbon-rich interstellar grains, including graphite, diamond, SiC, and TiC, have previously been found, isotopically anomalous interstellar oxide grains have proven more elusive. We have developed an ion imaging system which allows us to map the isotopic composition of large numbers of grains relatively quickly and is, thus, ideally suited to search for isotopically exotic subsets of grains. The system consists of a PHOTOMETRICS CCD camera coupled to the microchannel plate/fluorescent screen of the WU modified CAMECA IMS-3F ion microprobe. Isotopic images of the sample surface are focused on the CCD and digitized. Subsequent image processing identifies individual grains in the images and determines isotopic ratios for each. For the present work, we have imaged in O-16 and O-18; negligible contributions of (17)OH(-) and (16)OH2(-) signals to the O-18 signal allow the use of low mass resolution, simplifying the measurements. Repeated imaging runs on terrestrial corundum particles showed that the system measures isotopic ratios reproducibly to about +/- 40%. Each imaging run took about six minutes to complete, and for this study there were on average 5-15 grains in each image. We have conducted imaging searches in 2-4 micron size separates of both Orgueil and Murchison.

Nittler, L. R.↗

Chronology and isotopic geochemistry of apollo 14 basalts and Skaergard Gabbro, Eastern Greenland

Work completed on Apollo 14 basalts has been published. The two dates obtained from these rocks comprised the oldest and two of the three oldest ages (4.1 and 4.3 billion years) known for lunar maria basalts; thus their ages are important in understanding the moon's earliest history. Owing to the antiquity of these rocks, two more fragments have been dated as part of a second ASEE/NASA SFF program. The new ages are 3.95 and 4.12 billion years, thus further establishing and amplifying the earlier results. This work, although perhaps more interesting for its chronologic information, was begun as a test of chemical and petrographic models. Fragments of Apollo basalt were placed into five categories, based on petrologic and chemical, especially rare-earth element, composition. Isotopic studies were begun in an attempt to determine if the five groups of basalts were related by age or initial isotopic composition (isotopic composition of lava at time of extrusion). Although a few of the representatives of the five groups have the same age and/or initial strontium-isotopic composition, within the analtytical uncertainties, most apparently are unrelated. Petrologic implications of these data will be published in an appropriate journal.

Dasch, E. J.↗

Perspectives on Few-Body Cluster Structures in Exotic Nuclei

It is a fascinating phenomenon in nuclear physics that states with a pronounced few-body structure can emerge from the complex dynamics of many nucleons. Such halo or cluster states often appear near the boundaries of nuclear stability. As such, they are an important part of the experimental program beginning at the Facility for Rare Isotope Beams (FRIB). A concerted effort of theory and experiment is necessary both to analyze experiments involving effective few-body states, as well as to constrain and refine theories of the nuclear force in light of new data from these experiments. Here, as a contribution to exactly this effort, this paper compiles a collection of “perspectives” that emerged out of the Topical Program “Few-body cluster structures in exotic nuclei and their role in FRIB experiments” that was held at FRIB in August 2022 and brought together theorists and experimentalists working on this topic.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Volatile Element Evidence of Local MORB Mantle Heterogeneity Beneath the Southwest Indian Ridge, 48°–51°E

Abstract The mantle source beneath the Southwest Indian Ridge (SWIR) reflects a complex history of contamination. Magmatic volatile contents are vital tracers of these kinds of heterogeneities, which may fractionate otherwise constant volatile/non‐volatile elemental ratios, such as the H 2 O/Ce ratio. Although several studies have recently used trace element and isotopic data to address mantle source heterogeneity and magmatic processes at SWIR 48°–51°E region, volatile element constraints provide a valuable test of models for the origins of mantle heterogeneities in this region. Here, we present new data for nine rare basaltic glass samples from the 48°–51°E region, which enable careful assessment of the effects of primary versus secondary processes on the glass volatile contents. These samples are strongly affected by variable extents of carbon degassing, and shallow assimilation of Cl‐rich fluid, but also reveal consistently high H 2 O/Ce ratios (458.8 ± 14.9), among the highest in MORBs, that cannot be explained by late‐stage secondary processes, crustal assimilation, or simple melting of peridotite mantle at variable depths. Instead, the high H 2 O/Ce ratios are features of the mantle source composition. The 48°–51°E region is notably more depleted in highly incompatible trace elements relative to other regions of the SWIR, although this depletion is not apparent in H 2 O, which is similarly abundant throughout the SWIR. We link the high H 2 O/Ce ratios in these glasses with other trace element characteristics diagnostic of subduction and fluid addition, suggesting that the mantle source reflects signatures of a refractory mantle residue that previously melted within a subduction zone.

Wang, Wei↗

LaRC-developed catalysts for CO2 lasers

Pulsed CO2 lasers have many remote sensing applications from space, airborne, and ground platforms. The NASA Laser Atmospheric Wind Sounder (LAWS) system will be designed to measure wind velocities from polar earth orbit for a period of up to three years. Accordingly, this and other applications require a closed-cycle pulsed CO2 laser which necessitates the use of an efficient CO-O2 recombination catalyst for these dissociation products which otherwise would degrade the laser operation. The required catalyst must not only operate at low temperatures but also must operate efficiently for long time periods. The research effort at NASA LaRC has centered around development and testing of CO oxidation catalysts for closed-cycle, pulsed, common and rare-isotope CO2 lasers. Researchers examined available commercial catalysts both in a laser and under simulated closed-cycle laser conditions with efforts aimed toward a thorough understanding of the fundamental catalytic reaction. These data were used to design and synthesize new catalyst compositions to better meet the catalyst requirements for closed-cycle pulsed CO2 lasers. Syntheses and test results for catalysts developed at Langley Research Center which have significantly better long-term decay characteristics than previously available catalysts and at the same time operate quite well under lower temperature conditions are discussed.

Upchurch, Billy T.↗

Light-driven hydrogen evolution via a novel pincer/no pincer mechanism including a possible concerted proton electron transfer

The road to efficient molecular catalysts for artificial photosynthesis requires a great deal of basic research to address the challenges of anthropogenic global warming. An unexpected result of such research is a novel pincer/no pincer mechanism discovered for the DFT-calculated catalytic cycle of PNP-C2 complexes. Structural parameters from theoretical modeling are supported by single crystal X-ray data for the corresponding complexes. Using the examples of [M(II)Cl(PNP-C2-R)] + (M = Pd 2+ , Ni 2+ ; R = CH 3 , H; PNP-C2 = N,N-bis{(di(2-methoxy-phenyl)phosphanyl)ethyl}-N-alkylamine) this pincer/no pincer mechanism is supported by differential pulse voltammetric, cyclic voltammetric, UV-Vis spectroscopic (combined with voltammetry) and 31 P nuclear magnetic resonance spectroscopic studies. The efficiency of hydrogen evolution during artificial photosynthesis depends significantly on the ratio of photosensitiser and water reduction catalysts. At first sight, the results from irradiation experiments (gas chromatography and mass spectrometry) seem obvious, but show a considerable impact of secondary and tertiary amines within the pincer structure. The best result obtained for the palladium pincer complex was with a secondary amine as a proton relay, delivering a turnover number of 2237 after only 2.5 hours. In contrast the analogous water reduction catalyst with a methylated (tertiary) amine instead of a secondary one gives only 972 turnovers under the same experimental conditions, over the same time. For all photocatalytic measurements the amount of hydrogen is approximately 2.5-times higher when a secondary amine is used as the proton relay. The influences of these different amines on the activity of water reduction catalysts during irradiation experiments in H 2 O or D 2 O lead to evidence of a kinetic isotope effect, supporting a possible concerted proton electron transfer. DFT calculations of reaction enthalpies, activation energies and intrinsic reaction coordinates of the catalytic cycle support the high efficiency of the presented catalysts. In particular, results from secondary amines suggest new candidates as examples of the rarely known concerted proton electron transfer.

14 SOLAR ENERGY↗