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Measurements of Argon-39 from locations near historic underground nuclear explosions

Measurement of radioactive gas seepage from an underground nuclear explosion is one of the primary methods to confirm whether an event was nuclear in nature. Radioactive noble gas indicators that are commonly targeted by such measurements (e.g. 133Xe, 37Ar) have half-lives of 35 days or less. Argon-39, an activation product similar to 37Ar, is produced by the interaction between neutrons and potassium in the surrounding geology and has a half-life of 269 years. Measurements taken at three sites near three historic underground nuclear test locations at the Nevada National Security Site have all shown highly elevated levels of 39Ar in subsurface air decades after the test events. Elevated levels of 39Ar (30-50 times background) were also detected in atmospheric air collected roughly 30 cm above ground level near two of these sites, and outside the entrance of the one tunnel site. These measurements demonstrate that 39Ar has the potential to be a long-term signature of an underground nuclear event which can be reliably detected at the surface or in the shallow subsurface. This radionuclide detection of an underground nuclear event decades after the event takes place is in contrast to the commonly held assumption that detecting underground nuclear events via radionuclides at the surface needs to be done in a matter of months. Depending upon what further studies show about the robustness of this signature in a variety of geological settings, it may in fact be easy to detect underground nuclear events at the surface for a very long time post-detonation.

Johnson, Christine M.↗

The impact of tritium phytoremediation on plant health as measured by fluorescence

Phytoremediation, using plants for soil, sediment, or water contaminant clean-up, is an established technology dependent on plant health. Tritium (3H), a radioactive isotope of hydrogen that is generally found in the environment as tritiated water (HTO), is a low-level beta emitter with a half-life of 12.32 years. Chlorophyll fluorescence (CF) for monitoring risk assessment of tritium to plant health was conducted at the Tritium Irrigation Facility (TIF) located on the US Department of Energy's Savannah River Site (SRS) near Aiken, SC. Two fluorometers were evaluated in conjunction with phytoremediation at the 25 –acre TIF where tritiated groundwater is being spray–irrigated on a mixed coniferous/deciduous forested watershed as a means of reducing tritium release to a nearby stream that serves as a tributary to the Savannah River. Tritium activity in irrigated water averaged 104 + 42 pCi mL -1 during the 2003 project. Fluorescence parameters measured by the two fluorometers were well correlated with each other (p < 0.0001). Tritium in water respired from oak leaves ranged up to 1845.13 pCi ml -1 and 2138.22 pCi ml -1 in pine needles. Trees in both the test and control sites were approximately 15 years old. In this report we demonstrated that fluorescence parameters provide an effective way to estimate the impact of HTO on plant health in a noninvasive, extremely rapid, and cost-effective manner. In the current study applying fluorometry, plants within the TIF phytoremediation site exposed to the site tritiated water were not significantly impacted by the tritium phytoremediation based on CF parameters as compared to the control, a nascent non-irrigated site.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

Mechanistic calculation of the effective silver diffusion coefficient in polycrystalline silicon carbide: Application to silver release in AGR-1 TRISO particles

The silicon carbide (SiC) layer in tristructural isotropic (TRISO) fuel particles serves as a barrier to prevent the escape of fission products produced and not retained in the fuel kernel. The release of silver (Ag) is a concern due to the long half-life of the 110m Ag isotope. However, accurately determining the fission gas release rate requires knowing the diffusion coefficient through the SiC layer. In this study, we leverage atomistic calculations of Ag diffusivity in SiC bulk and grain boundaries (GBs) to develop a mesoscale effective Ag diffusion coefficient (D eff ) in SiC. Since GBs serve as pathways for Ag diffusion, D eff is defined as a function of temperature and microstructure variables. In particular, the size of SiC grains in the direction perpendicular to diffusion is shown to significantly affect Ag diffusion. The prediction of the mechanistic, mesoscale approach falls within one order of magnitude of empirical values. The temperature and microstructure-dependent effective Ag diffusivity in SiC is implemented in the fuel performance code Bison with a correction factor to predict Ag release from AGR-1 TRISO fuel particles. We hereby quantify the impact of SiC grain size on Ag release and improve Bison’s predictions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Multiscale, mechanistic modeling of irradiation-enhanced silver diffusion in TRISO particles

Tristructural isotropic (TRISO) particles are under consideration for use in several proposed advanced nuclear reactor concepts. The silicon carbide (SiC) layer in TRISO acts as a barrier to prevent the release of the fission products. However, despite remarkable retention, silver (Ag) release has been observed from intact particles, which requires investigation since the Ag isotope ( 110m Ag) has a long half-life. Previous work focused on developing a multiscale, mechanistic model for Ag diffusion accounting for temperature and microstructure effect and has been successfully validated. In this work, we expand the previous model to account for irradiation-enhanced Ag diffusivity in SiC and improve its accuracy over a wider grain size and temperature ranges relevant for advanced reactor conditions. A temperature, grain size, and flux dependent diffusivity is therefore derived using the mesoscale code MARMOT and implemented in the fuel performance code BISON. The irradiation-enhanced Ag diffusivity in SiC is compared against experimental data and validated using BISON against Ag release measurements from the Advanced Gas Reactor Fuel Development and Qualification Program (AGR-1 and AGR-2). Herein, we quantify the impact of SiC grain size, irradiation, and temperature on Ag release. In agreement with previous studies, we find accounting for SiC grain size improves agreement between BISON predictions and experimental observations for most cases. In conclusion, we also find that accounting for irradiation improves agreement for cases where Ag release was underestimated, but the impact was less significant than accounting for microstructure.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Evaluation of AGR-3/4 In-pile Silver Release Predictions Against Post-Irradiation Examination Measurements

Fuel performance modeling codes that accurately predict the transport of radionuclides in high-temperature gas-cooled reactors that utilize tristructural isotopic (TRISO) fuel particles are an important aspect of reactor safety analyses. One objective of the Advanced Gas Reactor (AGR)-3/4 experiment was to assess the transport of fission products through fuel particles and their subsequent release into the compact matrix and structural graphite materials. This was accomplished by irradiating uranium oxycarbide (UCO) driver fuel particles and designed-to-fail (DTF) particles to serve as known sources of fission products. The fission product of particular interest when it comes to such transport is silver (Ag-110 m), as it has a 250-day half-life and has relatively high mobility in the TRISO coating layers. Furthermore, to assess the current modeling capabilities and diffusion parameters employed in the fuel performance codes PARFUME and BISON, the fractional release of silver release predicted by the two codes were compared against post-irradiation examination measurements from the AGR-3/4 experiment.

AGR-3/4 Experiment↗

Striking stability of a mixed-valence thallium(III)-thallium(I) complex in some solvents

At the dissolution of solid anhydrous thallium(III) trifluoromethanesulfonate, Tl(CF 3 SO 3 ) 3 , or thallium(III) trifluoroacetate, Tl(CF 3 COO) 3 , in dimethylsulfoxide (dmso) or N,N,N’,N’-tetramethylurea (tmu), intensely red-colored complexes are formed. This red thallium complex is stable for years in dmso, while it is reduced fairly rapidly to thallium(I) in tmu with a half-life time of an hour. At the dissolution of Tl(CF 3 SO 3 ) 3 in N,N-dimethylpropyleneurea (dmpu) an immediate reduction to thallium(I) takes place. A stable colorless aqueous thallium(III) solution is obtained at the dissolution in acidic water. Stable dmso solutions and solid dmso solvates of thallium(III) perchlorate, nitrate and trifluormethanesulfonate can be prepared by adding dmso to concentrated acidic aqueous thallium(III) solutions. These experimental observations conclude that the pure solids Tl(CF 3 SO 3 ) 3 and Tl(CF 3 COO) 3 play an essential role in the formation of the red-colored thallium complexes. 205 Tl NMR data show that the red thallium complex contains equal amounts of thallium(III) and thallium(I). The structure of the red thallium complex in dmso, as determined by EXAFS, has Tl–O bond distances of 2.216(3) and 2.80(2) Å, which are in very close agreement with the bond distances obtained in the pure dmso solvates of the thallium(III) and thallium(I) ions, respectively, and a Tl···Tl distance of 3.49(1) Å bridged by oxygen atoms. From the EXAFS data it is impossible to distinguish if dmso molecules and/or trifluoromethanesulfonate ions act as bridges. DFT calculations could eliminate some structures due to the irrelevant structural parameters or the energetics of the proposed reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

New class of tritium breeders for fusion applications: Metal-reinforced composite breeders

Commercial fusion reactors operating on a D-T fuel cycle will require a steady supply of tritium to maintain the burning plasma required for continuous power generation. Since tritium has a short half-life, there is negligible natural abundance which necessitates fusion reactors to produce their own source of tritium. Tritium is most easily produced by surrounding a fusion reactor core with lithium (Li), which reacts under the intense neutron flux leaving the reactor core to form tritium and helium. Due to the hazards and technical challenges associated with surrounding a fusion reactor core with many tons of molten Li, other Li-bearing tritium breeder materials have been pursued. Unfortunately, most of the liquid breeders historically examined are exceedingly corrosive to reactor structural materials while many solid breeders in the form of ceramics are forced to make tradeoffs between Li content and mechanical integrity. In this work, to break the historic limit between Li-density and mechanical integrity of traditional solid breeders, a new class of solid tritium breeders is developed: metal-reinforced composite (MERC) breeders. Specifically, the high Li-density of lithium oxide (Li 2 O) is exploited through the addition of a metal reinforcing phase, producing a composite breeder material exhibiting high splitting tensile strength and quasi-ductility with a Li-density greater than other leading solid breeder candidates, including lithium orthosilicate (Li 4 SiO 4 ) and lithium metatitanate (Li 2 TiO 3 ). Mechanical testing, microstructural characterization, and neutronic simulation results are presented and discussed in light of fusion reactor design considerations.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Nuclear Data Sheets for A=190

The evaluated experimental data are presented and evaluated for 15 known nuclides of mass 190 (Hf, Ta, W, Re, Os, Ir, Pt, Au, Hg, Tl, Pb, Bi, Po). This work supersedes earlier full evaluations of A=190 by 2003Si05, 1990Si09, 1982Le22 and 1973Sc42. For 190Hf, only the isotopic identification has been made, with no information about the half-life of the ground state or its decay properties. For 190 Ta, only one excited state as an isomer has been identified, but with no knowledge about its decay properties. For 190 W, 190 Re, 190 Bi and 190 Po, available spectroscopic data are scarce. Here, the decay schemes of 190 Ta, 190 W, 190 Au, 190 Hg, 190 Au isomer decay, 190 Tl (both the activities), 190 Pb, and 190 Bi (both the activities) are considered incomplete by the evaluators. At present, extensive level structures, both the low-spin and high-spin, are known for 190 Os, 190 Ir, 190 Pt, 190 Au, 190 Hg, 190 Tl and 190 Pb, but data for level lifetimes, and γ-ray transition probabilities are generally lacking.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Nuclear Structure and Decay Data for A=31 Isobars

Here, experimental nuclear spectroscopic data are evaluated for 11 known nuclides of mass 31 (F, Ne, Na, Mg, Al, Si, P, S, Cl, Ar, K). Detailed evaluated information is presented for each reaction and decay experiment. Combining all the available data, recommended values are provided for energies, spins and parities, and half-lives of levels, with energies, branching ratios and multipolarities of γ radiations, and characteristics of β and α radiations in radioactive decays. 31 P is the most extensively studied one among all nuclides via various reactions and decays, followed by 31 S, 31 Si, 31 Mg and 31 Al. Information for excited states in 31 Ne, 31 Na, 31 Cl, 31 Ar and 31 K are limited; no excited states have yet been identified in 31 F, even its ground-state half-life is unknown. Significant new data have become available for the structure of 31 S, with its relevance to astrophysical applications. This work supersedes the earlier evaluation of A=31 by 2013Ou01, with literature cutoff date of Feb 15, 2013.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Nuclear Structure and Decay Data for A=71 Isobars

Experimental nuclear spectroscopic data are evaluated for 12 known nuclides of mass number=71 (Mn, Fe, Co, Ni, Cu, Zn, Ga, Ge, As, Se, Br, Kr). Detailed compiled and evaluated information is presented for each reaction and decay experiment. The β – n decay of 72 Co to 71 Ni is included in this work, while for β – n decay of 71 Co to 70 Ni, consult Nuclear Data Sheets for A=70 (2016Gu11) or the ENSDF database for 70 Ni. Combining all the available data, recommended values are provided for energies, spins and parities, and half-lives of levels, with energies, branching ratios and multipolarities of γ radiations, and characteristics of β and α radiations in radioactive decays. Excited-states have not yet been identified in 71 Mn, 71 Fe, and 71 Kr, with the ground-state half-life remaining unknown only for 71 Mn; data for excited states in 71 Co and 71 Ni are very limited; 71 Ga, 71 Ge and 71 As are the most extensively studied nuclides via various reactions and decays, followed by 71 Cu, 71 Zn, 71 Se, and 71 Br, however, except for 71 Ge, the decay schemes of all other nuclides are considered as incomplete due to a large gap between the decay Q-value and the highest observed level. Lastly, this work supersedes earlier evaluations of A=71 by 2011Ab01.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Nuclear Structure and Decay Data for A=44 Isobars

Experimental nuclear spectroscopic data are evaluated for 12 known nuclides of mass number A=44 (Si, P, S, Cl, Ar, K, Ca, Sc, Ti, V, Cr, Mn). Detailed evaluated information are presented for each reaction and decay. Recommended values combining all available data are provided for all spectroscopic properties of each level, γ-ray, and decay radiation. No excited states have yet been identified in 44 Si, 44 P, 44 Cr, and 44 Mn. Information for excited states in 44 Cl and 44 V are limited. Nuclides of 44 S, 44 Ar and 44 K have been studied via only a few reactions and decays, while 44 Ca, 44 Sc and 44 Ti are the most investigated nuclides through various reactions and decays. Evaluators note that the half-life of the g.s. of 44 S has been measured independently, with fairly good statistics, in three references, most precise being 100 ms 1 by 2004Gr20, but this value is in disagreement with the values of 125.5 ms 25 and 119 ms 6 by 2022Tr03, and 123 ms 10 by 1995So03. We adopted the unweighted average of this discrepant dataset. Another outstanding issue is that of the β + -delayed proton decay of 44 Cr g.s. to 44 V, where the T=2, 0 + IAS state in 44 V is expected to be strongly populated by a superallowed β transition, but has not been definitely identified as discussed in detail by 2020Fu05. A detailed study of 44 Cr decay is required to unravel the status of the T=2, 0 + IAS state in 44 V. Furthermore, this work supersedes earlier ENSDF evaluations of A=44 by 2011Ch39 and 1999Ca45.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Nuclear Structure and Decay Data for A=167 Isobars

Experimental nuclear spectroscopic data are compiled and evaluated for 17 known nuclides of mass 167 (Sm, Eu, Gd, Tb, Dy, Ho, Er Tm, Yb, Lu, Hf, Ta, W, Re, Os, Ir, Pt), 23 years after the previous full evaluation by 2000Ba65. Detailed information is presented for each reaction and decay experiment. Combining all the available data, recommended values are provided for energies, spins and parities, and half-lives of levels, with energies, branching ratios and multipolarities of γ radiations, and characteristics of β and α radiations in radioactive decays. Here, the α decays of A=171 nuclei to A=167 daughters are included in this work, while for α decays of A=167 nuclei to A=163 daughters, consult Nuclear Data Sheets (2010Re03) or the ENSDF database for A=163. 167 Er, 167 Tm, 167 Yb, 167 Lu and 167 Ta are among the most extensively studied nuclides via decay and high-spin gamma-ray spectroscopy measurements, followed by 167 Ho, 167 Hf, 167 W, and 167 Os. Information for excited states in 167 Dy, 167 Re, and 167 Ir are limited; no excited states have yet been identified in 167 Sm, 167 Eu, 167 Gd, 167 Tb and 167 Pt, with the ground-state half-life of 167 Sm remaining unknown. This work supersedes the earlier evaluation of A=167 nuclei by 2000Ba65.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

237 Np Fission Spectrum Cumulative Fission Product Yield Measurement Using Godiva IV Critical Assembly

Precise integral measurement of fast neutron-induced fission product yields for various actinides is of high interest for applied nuclear science. The goal of this effort is to improve uncertainties in fission product yield values of 237 Np. Fission was induced in a NpO 2 (NO 3 ) target using the Godiva IV critical assembly in burst mode. The irradiated sample was transferred to a high-resolution γ-ray detection setup within 50 minutes. γ-ray list mode data was collected from 50 minutes to 1 week after the irradiation. γ-ray spectroscopy was performed to analyze the time dependent γ-ray yields using an automated peak search algorithm to identify isotopes by their decay γ-ray energy and half-life. Finally, the initial activity for each isotope identified was used to calculate their fission product yield.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

239 Pu Fission Spectrum Cumulative Fission Product Yield Measurement Using Godiva IV Critical Assembly

Precise integral measurement of fast neutron-induced fission product yields for various actinides is of high interest for applied nuclear science. The goal of this effort is to improve uncertainties in fission product yield values of 239 Pu. Fission was induced in a pure 239 Pu (>99%) target using the Godiva IV critical assembly in burst mode. Further, the irradiated sample was transferred to a high-resolution γ-ray detector within 45 minutes. γ-ray list mode data was collected from 45 minutes to 1 week after the irradiation. γ-ray spectroscopy was performed to analyze the time dependent γ-ray yields using an automated peak search algorithm to identify isotopes by their decay γ-ray energy and half-life. The initial activity for each isotope identified was used to calculate their fission product yield.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Beta-delayed charged-particle spectroscopy using TexAT

β-delayed charged-particle emission is a sensitive probe of three-body decays in light nuclei. Time Projection Chambers (TPCs) offer a significant advantage over traditional charged-particle spectroscopy techniques due to a low-energy threshold and a high-geometric efficiency (≈ 4π) which are essential for use with radioactive ion beams where the beam intensities are limited. The technique for high-sensitivity spectroscopy of β-delayed charged-particle emission is shown to be possible using the Texas Active Target (TexAT) TPC in conjunction with the General Electronics for TPCs (GET) system. The benchmark case studied was that of 12 N β-decay to the first α-unbound state in 12 C, the Hoyle state. Here, half-life and branching ratio measurements are presented and are in good agreement with previous studies. The efficacy of using TPCs to study such a near-threshold state and disentangle the three-body dynamics of the decay products is demonstrated.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Distinguishing fissile uranium isotopes using an active well neutron coincidence counter

Proposed thorium-based nuclear fuel cycles are likely to require quantification and verification of 233 U within nuclear material. Because of their similar fission cross sections, active neutron nondestructive assay (NDA) systems may respond similarly to 233 U and 235 U. Traditional safeguards equipment has been optimized for 235 U and 238 U quantification associated with conventional uranium/plutonium fuel cycles and may not be directly applicable to 233 U quantification when mixed with other actinides. This work used models of the large volume active well coincidence counter (LV-AWCC) at Oak Ridge National Laboratory to evaluate the performance of this neutron NDA system to differentiate fissile uranium isotopes. The models were developed to simulate NDA system performance in response to a number of triangular radiation signature training device sources within the central cavity or well. This work predicted that the LV-AWCC can effectively differentiate 233 U from 235 U in certain modes of operation. In active mode, the LV-AWCC with the cadmium liner results in different doubles count rates between the fissile isotopes for a given fissile uranium mass. Without the cadmium liner, the uranium isotopes provide a statistically indistinguishable doubles count rate response for the fissile masses considered in this work (up to approximately 150 g). The cadmium liner serves to harden the neutron interrogation spectrum, which better exploits the notable difference in the 233 U and 235 U fission cross sections at approximately 1 eV. In passive mode, the two fissile isotopes exhibit different doubles and singles count rates regardless of liner presence because the passive source strength of 233 U is approximately 2 orders of magnitude stronger than that of 235 U due to the shorter half-life and correspondingly higher (α, n) yield. We conclude that using neutron interrogation in the LV-AWCC, two measurements are needed to quantify 233 U content in mixed uranium items. The first measurement is used to determine the total fissile uranium mass using a mode that cannot distinguish fissile isotopes (i.e., where a similar response is observed for both fissile uranium isotopes such as active doubles without cadmium or using a thermal neutron interrogation source). In conclusion, the second measurement is used to determine the 233 U content by using a differentiating technique (e.g., passive doubles, passive doubles to singles ratio, active doubles with cadmium).

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Off-line commissioning of the St. Benedict radiofrequency quadrupole cooler-buncher

The St. Benedict ion trapping system, which aims to measure the β - v angular correlation parameter in superallowed-mixed mirror transitions, is under construction at the University of Notre Dame. These measurements will provide much-needed data to improve the accuracy of the V ud element of the CKM matrix. One of the major components of this system is the radio frequency quadrupole cooler-buncher, which is necessary to create low-emittance ion bunches for injection into the measurement Paul trap. The off-line commissioning of the cooler-buncher, using a potassium ion source, determined that the device could produce cooled ion bunches characterized by a 50-ns full-width-half-maximum time width at its exit. The commissioning results also determined the trapping efficiency to be 93(1)% and the trapping half-life to be 20.0(5) s.

Paul trap↗

LaBr 3 : Ce self-activation analysis for measuring fast neutron fields

Measurement of the fast neutron production rate in deuterium–tritium (D–T) fusion reactions is important for applications such as active interrogation, fusion diagnostics, and borehole logging. Such measurements are typically performed by neutron activation analysis of metal foils, especially copper. Copper foil activation analysis requires efficiency and energy calibrations of the detector used to measure the foil, and it relies on the detection of 511 keV gamma rays, which are prominent in the active background when neutrons are being produced. Alternatives, such as 79m Br produced by inelastic neutron scattering on 79 Br, are limited by short half-life, low-energy gamma emission, and inability to selectively measure D–T neutrons. This work describes a novel alternative approach to measure ≳10 MeV neutron fields based on self-activation analysis of a LaBr 3 :Ce detector. The activity of 78 Br, the activation product of the 79 Br(n,2n) 78 Br reaction, is used to determine the neutron flux and infer the neutron production rate. We experimentally demonstrate the method with a cylindrical LaBr 3 :Ce crystal with a diameter and height of 3.81 cm that was placed at an ~18 cm distance from the neutron production point, at a 90° angle with respect to the deuteron beam in a D–T neutron generator. Operating voltage and current of the generator were adjusted to evaluate the technique’s performance over a nominal generator output range of approximately (1 - 9) x 10 7 n/s. The neutron output obtained from LaBr 3 :Ce activation agrees to within three standard deviations of the output obtained using copper activation. The self-activation technique can be conveniently employed in a variety of applications to simplify measurements of fast neutrons produced in D–T fusion reactions.

Active interrogationLaBr3↗