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At least 73 records · Page 4

Design Report on the MiniFuel Instrumented Test Apparatus for Understanding Radiation Effects

Most nuclear fuels irradiations at Oak Ridge National Laboratory (ORNL) over the past decade have been conducted using MiniFuel—a static capsule design employing subscale fuel specimens to collect separate-effects irradiated fuel performance data. Irradiation conditions for MiniFuel experiments are predicted pre-test using reactor physics, and thermal models are verified post-irradiation via SiC dilatometry and various spectrometry methods. Relevant fuel performance parameters are also observed post-irradiation in a hot cell, thereby providing a single data point for each parameter representing the cumulative effects of the irradiation conditions. Substantially more data can be harvested from a single test and within a shorter duration by instrumenting irradiation vehicles and measuring desired quantities in situ. This report presents the design and analysis of the MiniFuel INstrumented Irradiation Test Apparatus for Understanding Radiation Effects (MINITAURE)—an instrumented test rig based on the separate-effects MiniFuel concept that aims to capture fission gas release (FGR) and thermal conductivity degradation of fuel specimens during irradiation in the High Flux Isotope Reactor (HFIR). MINITAURE will be integrated with the Materials Irradiation Facility (MIF) located in the HFIR building outside the reactor containment. The MIF will act as the instrumentation and control center for the experiment, enabling real-time feedback from in situ sensors and control of irradiation temperatures via a gas delivery system. Two unique capsule designs were developed to capture each phenomenon: the thermal conductivity capsule, which uses a thermopile method to estimate fuel specimen thermal conductivity, and the fission gas release capsule, which will have continuous flowing gas communication to high-purity germanium detectors that are housed in the MIF for monitoring FGR. This report details the reactor physics and heat transfer modeling activities that were used to inform the experiment design and predict capsule performance. It also describes out-of-pile activities conducted to stand up this new capability and verify the measurement techniques. Modeling efforts to date have demonstrated the feasibility of the in situ measurement techniques and supported the development of the MINITAURE assembly configuration. Out-of-pile testing of the thermal conductivity measurement shows promise in capturing relative changes in thermal conductivity. However, significant errors exist in the measured absolute value, posing a need for further refinement.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Investigation of the 244 Pu ⁢( 48 Ca,𝑥⁢𝑛) 292−𝑥 Fl reaction with the LBNL SHREC detector: Investigation of decay chains of isotopes of flerovium (𝑍=114)

The 244 Pu ⁢( 48 Ca,𝑥⁢𝑛)⁢ 292−𝑥 Fl reaction was investigated at Lawrence Berkeley National Laboratory’s 88 Inch Cyclotron using the Berkeley Gas-filled Separator (BGS), the newly installed Superheavy Recoil detector, along with an upgraded digital electronics and data acquisition system. Seven decay chains were observed starting with an evaporation residue, followed by a single 𝛼 decay and a spontaneous fission. The decay characteristics of these seven decay chains led to an assignment to 288 Fl , the product of the 4⁢𝑛 reaction channel. Two additional chains were (tentatively) assigned to the decay of the 3⁢𝑛 exit channel, 289 Fl . Cross sections for the 4⁢𝑛 and 3⁢𝑛 exit channels were 𝜎 prod =6.7⁢($^{36}_{25}$) pb and 𝜎 prod =1.6⁢($^{22}_{11}$) pb, respectively. Another decay chain, tentatively assigned to the 5⁢𝑛 exit channel through the 48 Ca + 244 Pu reaction or the 3⁢𝑛 exit channel of the 48 Ca + 242 Pu reaction, was also detected. Detailed information regarding the observed decay chains and their nuclear structure aspects is discussed, along with the performance of the BGS and the new detection system.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Oxygen isotope cosmothermometer.

Variations in oxygen isotopic abundances of meteoritic minerals, chondrules, whole meteorites, and planets are discussed in terms of a model involving isotopic exchange between primordial dust and a cooling solar nebular gas. From the temperature-dependence of the isotopic fractionation factors, temperatures have been assigned to the processes of initial condensation, chondrule formation, and planetary accretion. Separated phases from carbonaceous chondrites fall into three isotopic groups representing widely differing conditions of formation: (1) low-iron olivine and pyroxene, and calcium-aluminum silicates condensed at temperatures above 1000 K; (2) high-iron olivine and pyroxene melted to form chondrules after prior cooling and exchange to temperatures of 530-620 K; and (3) hydrous silicates condensed at temperatures below 400 K.

Onuma, N.↗

Colloidally separated samples from Allende residues - Noble gases, carbon and an ESCA-study

Results are presented which strengthen the hypothesis of heterogeneity among the carbon- and nitrogen-bearing phases of the Allende meteorite. These data also highlight the possibility of performing physical separations yielding samples in which some of the noble gas- and carbon-bearing phases are extraordinarily predominant over others. The conclusion, based on mass and isotope balance arguments, that a significant portion of the carbonaceous matter in Allende is likely to be gas-poor or gas-free need not weaken the case for carbonaceous carriers for the major noble gas components. The concept that acid-soluble carbonaceous phases contain a multiplicity of components, each of which may have formed under a multiplicity of different physical-chemical conditions, is reemphasized by the results of the present study.

Ott, U.↗

Noble-gas-rich separates from the Allende meteorite

Predominantly carbonaceous HF/HCl-resistant residues from the Allende meteorite are studied. Samples are characterized by SEM/EDXA, X-ray diffraction, INAA, C, S, H, N, and noble gas analyses. Isotopic data for carbon show variations no greater than 5%, while isotopic data from noble gases confirm previously established systematics. Noble gas abundances correlate with those of C and N, and concomitant partial loss of C and normal trapped gas occur during treatments with oxidizing acids. HF/HCl demineralization of bulk meteorite results in similar fractional losses of C and trapped noble gases, which leads to the conclusion that various macromolecular carbonaceous substances serve as the main host phase for normal trapped noble gases and anomalous gases in acid-resistant residues, and as the carrier of the major part of trapped noble gases lost during HF/HCl demineralization. Limits on the possible abundances of dense mineralic host phases in the residues are obtained, and considerations of the nucleogenetic origin for CCF-XE indicate that carbonaceous host phases and various forms of organic matter in carbonaceous meteorites may have a presolar origin.

Ott, U.↗

Hydrogen (H) Isotope Composition of Type II Kerogen Extracted by Pyrolysis-GC-MS-IRMS: Terrestrial Shale Deposits as Martian Analogs

Described here is a technique for H isotope analysis of organic compounds pyrolyzed from kerogens isolated from gas‐ and liquids‐rich shales. Application of this technique will progress the understanding of the use of H isotopes not only in potential kerogen occurrences on Mars, but also in terrestrial oil and gas resource plays. H isotope extraction and analyses were carried out utilizing a CDS 5000 Pyroprobe connected to a Thermo Trace GC interfaced with a Thermo MAT 253 IRMS. Also, a split of GC‐separated products was sent to a DSQ II quadrupole MS to make qualitative and semi‐quantitative compositional measurements of these products. Kerogen samples from five different basins (type II and II‐S) were dehydrated (heated to 80 C overnight under vacuum) and analyzed for their H isotope compositions by Pyrolysis‐GC‐MS‐TC‐IRMS. This technique takes pyrolysis products separated via GC and reacts them in a high temperature conversion furnace (1450 C), which quantitatively forms H2. Samples ranging from ~0.5 to 1.0mg in size, were pyrolyzed at 800 C for 30s. and separated on a Poraplot Q GC column. H isotope data from all kerogen samples typically show enrichment in D from low to high molecular weight. H2O average delta D = ‐215.2 per mille (V‐SMOW), ranging from ‐ 271.8 per mille for the Marcellus Shale to ‐51.9 per mille for a Polish shale. Higher molecular weight compounds like toluene (C7H8) have an average delta D of ‐89.7 per mille, ranging from ‐156.0 per mille for the Barnett Shale to ‐50.0 per mille for the Monterey Shale. We interpret these data as representative of potential H isotope exchange between hydrocarbons and sediment pore water during basin formation. Since hydrocarbon H isotopes readily exchange with water, these data may provide some useful information on gas‐water or oil‐water interaction in resource plays, and further as a possible indicator of paleoenvironmental conditions. Alternatively, our data may be an indication of H isotope exchange with water and/or acid during the kerogen isolation process. Either of these interpretations will prove useful when deciphering H isotope data derived from kerogen analyses. Understanding the role that these H‐bearing compounds play in terrestrial shale paleo‐environmental reconstruction may also prove useful as analogs for understanding the interactions of water and potential kerogen/organic compounds on the planet Mars.

Socki, Richard A.↗

Theoretical investigations of plasma processes

System analyses are presented for electrically sustained, collision dominated plasma centrifuges, in which the plasma rotates under the influence of the Lorentz forces resulting from the interaction of the current density fields with an external magnetic field. It is shown that gas discharge centrifuges are technically feasible in which the plasma rotates at speeds up to 1 million cm/sec. The associated centrifugal forces produce a significant spatial isotope separation, which is somewhat perturbed in the viscous boundary layers at the centrifuge walls. The isotope separation effect is the more pronounced. The induced magnetic fields have negligible influence on the plasma rotation if the Hall coefficient is small. In the technical realization of collision dominated plasma centrifuges, a trade-off has to be made between power density and speeds of rotation. The diffusion of sputtered atoms to system surfaces of ion propulsion systems and the deposition of the atoms are treated theoretically by means of a simple model which permits an analytical solution. The problem leads to an inhomogeneous integral equation.

Wilhelm, H. E.↗

Rare gas analysis of size fractions from the Fayetteville meteorite

Eight size separates of grains from the Fayetteville meteorite ranging from less than 20 microns to greater than 1 millimeter are being analyzed for their rare gas elemental and isotopic composition. Measurements on five samples were performed. All five reveal a mixture of solar, planetary, cosmic ray produced and radiogenic gases. The solar component is of particular interest since it suggest that the meteorite may represent a fragment of an ancient protoplanetary regolith which was exposed to the solar wind. Solar wind elements are implanted in the outer few hundred Angstroms of exposed grains and are therefore expected to be surface correlated. At present the data do not suggest that such a correlation exists, but the final conclusion must await further analyses and data reduction.

Jordan, Jim L.↗

Photonuclear Production of Radioxenon for Air Samples

Radioxenon plays an important role in ensuring compliance with the Comprehensive Nuclear-Test-Ban Treaty due to its ability to be transported through the atmosphere, as well as the fact that the half-lives of its isotopes provide a window long enough to be detected but not long enough that it could become background radiation. This allows it to be correlated with specific events that indicate the testing of nuclear weapons. Idaho National Laboratory supports this mission by providing spiked air samples for monitoring stations to enable instrument calibration and ensure measurement accuracy. We tested a photonuclear method of producing one of the main isotopes of radioxenon, Xe-135. We also tested the separation of Xe-135 from the parent isotope Xe-136 using the method of kinematic recoil. Aluminum coils were placed in quartz ampoules filled with enriched Xe-136 and were irradiated by a bremsstrahlung beam with an endpoint energy of 21 MeV. The results showed that we were not only successful in producing Xe-135 but also that the Xe-135 was deposited into the coil allowing it to be removed from the Xe-136 gas. The coil and the Xe-135 can then be chemically separated. At the time of counting the coil, it was calculated that there was about 18 Bq of activity from Xe-135 remaining in the coil. Future work includes determining the optimal material and geometry of the catcher to maximize the amount of Xe-135 captured.

07 ISOTOPE AND RADIATION SOURCES↗

A Simple Mechanism for Fractionating Oxygen Isotopes in the Solar Nebula

Lightning in the Solar Nebula is caused by the tribo-electric charging of dust grains carried by massive turbulent flows and driven by the accretion energy in the disk: it has long been one agent assumed responsible for the formation of chondrules. The degree to which charge separation can occur is dependent upon a number of factors, including the concentration of radioactive sources and the total level of ionization in the nebula, and these factors determine the maximum energy likely to be released by a single bolt. While chondrule formation requires a massive discharge, even a small lightning bolt can vaporize grains in the ionized discharge channel. Experimental studies have shown that silica, iron silicate and iron oxide grains formed from a high voltage discharge in hydrogen rich gas containing some oxygen produces solids that are enriched in O-17 and O-18 relative to the composition of the starting gas. Vaporization of silicates produces SiO, metal and free oxygen atoms in each discharge and these species will immediately begin to recondense from the hot plasma. Freshly condensed grains are incrementally enriched in heavy oxygen while the gas is enriched in O-16. Repeated evaporation and condensation of silicates in continuously occurring lightning discharges will monotonically increase the fractionation of oxygen isotopes between the O-17 and O-18 rich dust and the O-16 rich gas. The first mass independently fractionated refractory oxide particles were produced in the lab following the condensation of a flowing gas mixture containing variable amounts of hydrogen, silane, pentacarbonyl iron and oxygen that passed through a high voltage discharge powered by a Tesla coil. While the exact chemical pathway is still uncertain, the most probable reaction mechanisms involve oxidation of the growing refractory clusters by O3, OH or O atoms. This model has some interesting consequences for chemical processes in the early solar nebula. Chemical fractionation of recondensed dust evaporated via lightning discharges should be strongly time dependent. At earlier times, the accretion rate is maximal, thus driving strong turbulence, energetic grain-grain collisions, tribo-electric charging and charge separation, leading to frequent, powerful lightning discharges. As the accretion rate diminishes, turbulence decreases and lightning discharges will become both less powerful and less frequent, thus decreasing the rate of dust-gas fractionation. The most rapid increase in the formation of O-16 poor dust will occur early in nebular history. Generation of fractionated dust should be distributed throughout the inner disk. Once condensed, grain dispersal would average out any significant isotopic anomalies within the inner disk.

Nuth, Joseph A., III↗

A statistical approach to screening isotopic signatures in monitoring for underground nuclear explosions

The ability to differentiate between atmospheric radionuclide signatures from underground nuclear explosions (UNEs) and signals from other sources, such as medical isotope-production facilities and nuclear reactors, can be critical to the detection and monitoring of unannounced, low-yield nuclear events. Signatures having anomalously high amplitudes, compared to background levels, remain the best indicator in screening for a UNE. However, isotopic composition can further validate a suspected UNE signature, but separation from any atmospheric background composition is first necessary. To date, evaluating the challenges of performing this separation has typically involved comparing an observed background with a highly idealized deterministic model of radioxenon signature production by a UNE that does not consider the influence of post-detonation chemical/physical processes in the detonation cavity or the subsequent gas transport mechanisms that can also affect the isotopic composition of the detected gas signature. In addition, purely deterministic models, as previously employed, overlook the uncertainty inherent in estimating critical parameters characterizing the UNE and its detonation environment. In this paper, we create detailed, multi-parameter models of radionuclide evolution using the widely accepted England and Rider post-detonation radionuclide decay-chain network coupled to detailed models simulating physical production and transport processes affecting the gas signature. Because these models are governed by uncertain parameters including barometric fluctuations, realistic ranges of variation for each of the parameters influencing isotopic composition are then defined. A Latin-Hypercube sampling approach is used to obtain a random distribution of isotopic production and gas transport results associated with a given value of each parameter. We apply these results to background histories of two stations, one providing 4-isotope background measurements and the other providing two-isotope measurements associated with the 2013 DPRK announced UNE.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Isotope alpha irradiators for radiobiological research

Radiation absorption is considered for the case where the isotopic alpha source, in the form of a flat disk, and the axially located biological object, also in the form of a flat disk, are separated by a layer of gas. Frequently the biological object is covered by a polymer film with minimal thickness for protection against radioactive contaminants. The energy of the alpha particle is calculated at the place where the absorbed dose is determined, taking into account loss of energy in air, film and tissue. The level of energy is determined by the specific loss in energy of the alpha particle arriving from the point source to a point at the biological subject.

Drasher, V.↗

The relationship between carbon monoxide abundance and visual extinction in interstellar clouds

Carbon monoxide column densities are compared to visual extinctions toward field stars in the rho Oph and Taurus molecular cloud complexes. The relationship of C(0-18) column density to extinction is established, and new determinations for (C-13)O column densities are given for a range of visual extinctions extended to beyond 20 mag. A prescription for determining hydrogen column densities and masses of molecular clouds from observations of CO isotopes is presented and discussed critically. These measurements agree well with the predictions of gas phase chemistry models which include chemical fractionation and selective isotopic photodestruction. The functional dependence of the C(O-18) column density on extinction is characterized by two different regimes separated by a distinct transition observed to occur at 4 mag in both molecular cloud complexes, whereas the functional dependence of (C-13)O is quite different in the two regions. Some saturation is found to occur for C(O-18) emission at high visual extinction and use the rarer isotopic species C(O-17) and (C-13)(O-18) to correct for it.

Frerking, M. A.↗

Properties of the 256 Db decay chain

Experiments were performed at Lawrence Berkeley National Laboratory's 88-Inch Cyclotron Facility to study the decays of neutron-deficient dubnium isotopes. These isotopes were produced in the 206 Pb( 51 V, xn) 255,256 Db reaction, and excitation functions were measured. This article reports on the observed properties of the 256 Db decay chain. The produced 256 Db nuclei were separated from unreacted-beam material and reaction byproducts with the Berkeley Gas-filled Separator (BGS) before being implanted into a double-sided silicon strip detector at the BGS focal plane. Decay properties of 256 Db and its daughters were then extracted from the analysis of correlations between implanted Db nuclei with α decay chains and spontaneous fission (SF) events. In total, 86 decay chains and 38 SF events were observed, giving increased statistics as compared to previous studies. In conclusion, improved decay data are presented for 256 Db and its daughter isotopes 252 Lr, 252 No, 248 Md, 248 Fm, 244 Es, and 244 Cf.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

The dependence of confinement on the isotope mass in the core and the edge of AUG and JET-ILW H-mode plasmas

Experiments in ASDEX Upgrade (AUG) and JET with the ITER-like wall (JET-ILW) are performed to separate the pedestal and core contributions to confinement in H-modes with different main ion masses. A strong isotope mass dependence in the pedestal is found which is enhanced at high gas puffing. This is because the ELM type changes when going from D to H for matched engineering parameters, which is likely due to differences in the inter ELM transport with isotope mass. The pedestal can be matched in H and D plasmas by varying only the triangularity and keeping the engineering parameters relevant for core transport the same. With matched pedestals Astra/TGLF (Sat1geo) core transport simulations predict the experimental profiles equally well for H and D. These core transport simulations show a negligible mass dependence and no gyro-Bohm scaling is observed. However, to match the experimental observations at medium β it is required to take the fast-ion dilution and rotation into account. This is not enough for high β plasmas where for the first time a profile match between H and D plasmas was achieved experimentally. Under these conditions quasilinear modelling with TGLF over predicts the transport in the core of H and D plasmas alike.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Results of Speciation Determination Measurements of Insulating Sulfur Hexafluoride Gas

Under the direction of the NNSA NA-231 Mo-99 Program, SRNL has provided technical assistance to U.S. companies under cooperative agreements. One such area of technical assistance has been for the recommendation for contamination management methods in the eventuality that tritium contaminates the insulating gas of a high-voltage ion source used in the accelerator-based process developed by SHINE Medical Technologies to produce Mo-99. The SHINE accelerator process uses tritium as the target of a deuterium ion beam, where the ion beam is produced within a high-voltage ion source insulated with sulfur hexafluoride (SF 6 ), and is separated from the tritium target by an extensive pump train. Normal operating conditions preclude the conditions necessary for contamination of the insulating gas, however certain atypical conditions could result in a tritium contamination event. Accelerator based processes for medical isotope production represent an anomalous tritium contamination challenge due to the presence of SF 6 . SF 6 decomposes through normal use as an insulator gas, and the exact speciation of the decomposition byproducts depends on a variety of factors. This creates a scenario where the anticipation of species present in the insulating gas mixture is difficult. In turn, the fate of tritium within such a chemical system is unclear. This document discusses the results of measurements made in-situ of the SF 6 insulating gas in use within a SHINE Medical Technology’s high-voltage ion source. This was done in an effort to determine the chemical speciation of the gas, allowing for the recommendation of management strategies in the event that tritium contaminates the insulating gas. The results of the measurements reported in this work suggest that tritium contamination in the insulating gas may result in two chemical forms of tritium in the system, tritiated water and molecular tritium. These two forms of tritium would be captured by two methods. Tritiated water may be captured and removed from the SF 6 by an adsorbent canister already present within the pressure vessel that houses the insulating gas while in use. It may also be separated from the SF 6 during routine purification of the SF 6 , which is performed by SHINE personnel routinely. The purification cart will perform all non-embedded systems cleanup necessary to remediate tritiated species in the system. The purification cart passes the insulating gas through several filters, followed by the liquefication of the SF 6 . The filters will separate tritiated water from the SF 6 at this stage. It is expected that molecular tritium will accumulate in the gas-phase during the liquification step, which is separated and stored. Tritium may be recovered from this mixture through more conventional hydrogen purification methods such as a palladium diffuser.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Hydrogen Isotope Measurements of Organic Acids and Alcohols by Pyrolysis-GC-MS-TC-IRMS: Application to Analysis of Experimentally Derived Hydrothermal Mineral-Catalyzed Organic Products

We report results of experiments to measure the H isotope composition of organic acids and alcohols. These experiments make use of a pyroprobe interfaced with a GC and high temperature extraction furnace to make quantitative H isotope measurements. This work compliments our previous work that focused on the extraction and analysis of C isotopes from the same compounds [1]. Together with our carbon isotope analyses our experiments serve as a "proof of concept" for making C and H isotope measurements on more complex mixtures of organic compounds on mineral surfaces in abiotic hydrocarbon formation processes at elevated temperatures and pressures. Our motivation for undertaking this work stems from observations of methane detected within the Martian atmosphere [2-5], coupled with evidence showing extensive water-rock interaction during Mars history [6-8]. Methane production on Mars could be the result of synthesis by mineral surface-catalyzed reduction of CO2 and/or CO by Fischer-Tropsch Type (FTT) reactions during serpentization [9,10]. Others have conducted experimental studies to show that FTT reactions are plausible mechanisms for low-molecular weight hydrocarbon formation in hydrothermal systems at mid-ocean ridges [11-13]. Our H isotope measurements utilize an analytical technique combining Pyrolysis-Gas Chromatograph-Mass Spectrometry-High Temperature Conversion-Isotope Ratio Mass Spectrometry (Py-GC-MS-TC-IRMS). This technique is designed to carry a split of the pyrolyzed GC-separated product to a Thermo DSQII quadrupole mass spectrometer as a means of making qualitative and semi-quantitative compositional measurements of separated organic compounds, therefore both chemical and isotopic measurements can be carried out simultaneously on the same sample.

Socki, Richard A.↗

New proton emitter 188 At implies an interaction unprecedented in heavy nuclei

We report the discovery of a new atomic nucleus 188 At, which is the heaviest proton-emitting isotope known to date. The new activity was observed through the 107 Ag( 84 Sr, 3n) 188 At fusion-evaporation reaction using the focal-plane spectrometer of the gas-filled recoil separator in the Accelerator Laboratory of the University of Jyväskylä, Finland. To fully interpret the experimental data, we have expanded the non-adiabatic quasiparticle model to treat nuclei in the beyond-lead region. The description reproduced the measured decay rate and pointed towards emission from an extremely prolate-deformed state with a dominant s 1/2 proton component in the wave function. The Thomas-Ehrman shift can be enhanced in low angular momentum states, but such effects have not been observed in heavy nuclei. The single-proton separation energy of 188 At deviates from that extrapolated from the systematics, which can be interpreted as the first evidence of this effect in heavy nuclei.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗