Nanoscale heterogeneity induced by nonmagnetic Zn dopants in the quantum critical metal CeCoIn; In NQR/NMR and Co NMR study

Sakai, Hironori; Tokunaga, Yo; Kambe, Shinsaku; Zhu, J.-X.*; Ronning, F.*; Thompson, J. D.*; Ramakrishna, S. K.*; Reyes, A. P.*; Suzuki, Kohei*; Oshima, Yoshiki*; et al.

Physical Review B, 104(8), p.085106_1 - 085106_12, 2021/08

https://doi.org/10.1103/PhysRevB.104.085106

Antiferromagnetism in a prototypical quantum critical metal CeCoIn is known to be induced by slight substitutions of non-magnetic Zn atoms for In. In nominally 7% Zn substituted CeCoIn, an antiferromagnetic (AFM) state coexists with heavy fermion superconductivity. Heterogeneity of the electronic states is investigated in Zn doped CeCoIn by means of nuclear quadrupole and magnetic resonances (NQR and NMR). Site-dependent NQR relaxation rates indicate that the AFM state is locally nucleated around Zn substituents in the matrix of a heavy fermion state, and percolates through the bulk at the AFM transition temperature . At lower temperatures, an anisotropic superconducting (SC) gap below the SC transition temperature , and the SC state permeates through the AFM regions via a SC proximity effect. Applying an external magnetic field induces a spin-flop transition near 5 T, reducing the volume of the AFM regions. Consequently, a short ranged inhomogeneous AFM state survives and coexists with a paramagnetic Fermi liquid state at high fields.

Final report on feasibility study of Pu monitoring and solution measurement of high active liquid waste containing fission product at Reprocessing Facility

Sekine, Megumi; Matsuki, Takuya; Suzuki, Satoshi*; Tsutagi, Koichi; Nishida, Naoki; Kitao, Takahiko; Tomikawa, Hirofumi; Nakamura, Hironobu; LaFleur, A.*; Browne, M.*

JAEA-Technology 2019-023, 160 Pages, 2020/03

JAEA-Technology-2019-023.pdf:9.43MB

The International Atomic Energy Agency (IAEA) has proposed in its Research and Development plan (STR-385), the development of technology to enable real-time flow measurement of nuclear material as a part of an advanced approach to effective and efficient safeguards for reprocessing facilities. To address this, Japan Atomic Energy Agency (JAEA) has been tackling development of a new detector to enable monitoring of Pu in solutions with numerous FPs as a joint research program with U.S. DOE to cover whole reprocessing process. In this study, High Active Liquid Waste (HALW) Storage Facility in Tokai Reprocessing Plant was used as the test field. At first, the design information of HALW storage tank and radiation (type and intensity) were investigated to develop a Monte Carlo N-Particle Transport Code (MCNP) model. And then, dose rate distribution outside/ inside of the concrete cell where the HALW tank is located was measured to design new detectors and check MCNP model applicability. Using the newly designed detectors, gamma rays and neutron were continuously measured at the outside/ inside of the concrete cell to assess the radiation characteristics and to optimize detector position. Finally, the applicability for Pu monitoring technology was evaluated based on the simulation results and gamma-ray/neutron measurement results. We have found that there is possibility to monitor the change of Pu amount in solution by combination both of gamma-ray and neutron measurement. The results of this study suggested the applicability and capability of the Pu motoring to enhance safeguards for entire reprocessing facility which handles Pu with FP as a feasibility study. This is final report of this project.

Systematic measurements and analyses for lead void reactivity worth in a plutonium core and two uranium cores with different enrichments

Fukushima, Masahiro; Goda, J.*; Oizumi, Akito; Bounds, J.*; Cutler, T.*; Grove, T.*; Hayes, D.*; Hutchinson, J.*; McKenzie, G.*; McSpaden, A.*; et al.

Nuclear Science and Engineering, 194(2), p.138 - 153, 2020/02

https://doi.org/10.1080/00295639.2019.1663089

To validate lead (Pb) nuclear cross sections, a series of integral experiments to measure lead void reactivity worth was conducted systematically in three fast spectra with different fuel compositions on the Comet critical assembly of the National Criticality Experiments Research Center. Previous experiments in a high-enriched uranium (HEU)/Pb and a low-enriched uranium (LEU)/Pb systems had been performed in 2016 and 2017, respectively. A follow-on experiment in a plutonium (Pu)/Pb system has been completed. The Pu/Pb system was constructed using lead plates and weapons grade plutonium plates that had been used in the Zero Power Physics Reactor (ZPPR) of Argonne National Laboratory until the 1990s. Furthermore, the HEU/Pb system was re-examined on the Comet critical assembly installed newly with a device that can guarantee the gap reproducibility with a higher accuracy and precision, and then the experimental data was re evaluated. Using the lead void reactivity worth measured in these three cores with different fuel compositions, the latest nuclear data libraries, JENDL 4.0 and ENDF/B VIII.0, were tested with the Monte Carlo calculation code MCNP version 6.1. As a result, the calculations by ENDF/B-VIII.0 were confirmed to agree with lead void reactivity worth measured in all the cores. It was furthermore found that the calculations by JENDL 4.0 overestimate by more than 20% for the Pu/Pb core while being in good agreements for the HEU/Pb and LEU/Pb cores.

Pu nuclear magnetic resonance in the candidate topological insulator PuB

Dioguardi, A. P.*; Yasuoka, Hiroshi*; Thomas, S. M.*; Sakai, Hironori; Cary, S. K.*; Kozimor, S. A.*; Albrecht-Schmitt, T. E.*; Choi, H. C.*; Zhu, J.-X.*; Thompson, J. D.*; et al.

Physical Review B, 99(3), p.035104_1 - 035104_6, 2019/01

https://doi.org/10.1103/PhysRevB.99.035104

We present a detailed nuclear magnetic resonance (NMR) study of Pu in bulk and powdered single-crystal plutonium tetraboride (PuB), which has recently been investigated as a potential correlated topological insulator. The Pu NMR spectra are consistent with axial symmetry of the shift tensor showing for the first time that Pu NMR can be observed in an anisotropic environment and up to room temperature. The temperature dependence of the Pu shift, combined with a relatively long spin-lattice relaxation time (), indicate that PuB adopts a nonmagnetic state with gaplike behavior consistent with our density functional theory calculations. The temperature dependencies of the NMR Knight shift and imply bulk gaplike behavior confirming that PuB is a good candidate topological insulator.

CIELO collaboration summary results; International evaluations of neutron reactions on uranium, plutonium, iron, oxygen and hydrogen

Chadwick, M. B.*; Capote, R.*; Trkov, A.*; Herman, M. W.*; Brown, D. A.*; Hale, G. M.*; Kahler, A. C.*; Talou, P.*; Plompen, A. J.*; Schillebeeckx, P.*; et al.

Nuclear Data Sheets, 148, p.189 - 213, 2018/02

https://doi.org/10.1016/j.nds.2018.02.003

The CIELO collaboration has studied neutron cross sections on nuclides that significantly impact criticality in nuclear facilities - U, U, Pu, Fe, O and H - with the aim of improving the accuracy of the data and resolving previous discrepancies in our understanding. This multi-laboratory pilot project, coordinated via the OECD/NEA Working Party on Evaluation Cooperation (WPEC) Subgroup 40 with support also from the IAEA, has motivated experimental and theoretical work and led to suites of new evaluated libraries that accurately reflect measured data and also perform well in integral simulations of criticality. This report summarizes our results and outlines plans for the next phase of this collaboration.

Improvement of INVS measurement uncertainty for Pu and U-Pu nitrate solution

Swinhoe, M. T.*; Menlove, H. O.*; Marlow, J. B.*; Makino, Risa; Nakamura, Hironobu

LA-UR-17-23474, 28 Pages, 2017/04

https://doi.org/10.2172/1356101

The Inventory Verification Sample system (INVS) has been used for IAEA verification measurement at the Plutonium Conversion Development Facility for MOX powder and Pu solution samples (measurement uncertainty: about 3-5%). If the measurement uncertainty can be improved (to 1%), it is expected that the range of usage can be extended and it could reduce the number of destructive analyses. In order to improve the measurement uncertainty for solution samples, we conducted three different types of calibration method that are passive calibration curve method, known- method and multiplicity method after optimization of detector parameter and sample position. In the range of concentration of typical solution samples, a good correlation was found between measured doubles and Pu effective mass in the three methods. Especially, the result of the conventional calibration curve method and known- method met our target uncertainty within 1% (22 hours measurement). Since it is thought that background singles change may affect measurement uncertainty, an additional shielding was installed around the INVS to reduce those effects. This shielding improved measurement uncertainty in known- method. The results with this shielding suggests passive calibration method and known- method could achieve the target uncertainty within 1% less than 1 hour measurement time.

Field test and evaluation of He replacement technologies; Development of HLNB counter

Tanigawa, Masafumi; Mukai, Yasunobu; Nakamura, Hironobu; Kurita, Tsutomu; Henzlova, D.*; Menlove, H. O.*

Dai-37-Kai Kaku Busshitsu Kanri Gakkai Nihon Shibu Nenji Taikai Rombunshu (CD-ROM), 9 Pages, 2017/02

no abstracts in English

Field test of a full scale He-alternative HLNC-type counter; High Level Neutron counter-Boron (HLNB)

Henzlova, D.*; Menlove, H. O.*; Tanigawa, Masafumi; Mukai, Yasunobu; Nakamura, Hironobu

EUR-28795-EN (Internet), p.313 - 323, 2017/00

http://publications.jrc.ec.europa.eu/repository/bitstream/JRC107151/esarda_symposium_proceedings-final.pdf

Facing the depletion of He gas supply and the continuing uncertainty of options for future resupply, Los Alamos National Laboratory (LANL) designed and built a He free full scale thermal neutron coincidence counter based on boron-lined parallel-plate proportional technology. The counter was designed as a direct alternative to High Level Neutron Coincidence counter (HLNC-II). This paper provides a summary of performance evaluation of HLNB under realistic field conditions at Plutonium Conversion Development Facility (PCDF) of Japan Atomic Energy Agency (JAEA). The field test included a range of small to large mass MOX materials that represent realistic process samples and provided key insight on and validation of the feasibility of HLNB as a safeguards instrument in realistic facility environment. In particular, the results of verification measurements demonstrate that HLNB is capable to satisfy ITV expected for HLNC-II-type counter of 2.1% in 300s measurement time.

Thermal expansion measurement of (U,Pu)O in oxygen partial pressure-controlled atmosphere

Kato, Masato; Ikusawa, Yoshihisa; Sunaoshi, Takeo*; Nelson, A. T.*; McClellan, K. J.*

Journal of Nuclear Materials, 469, p.223 - 227, 2016/02

https://doi.org/10.1016/j.jnucmat.2015.11.048

Thermal expansion of (UPu)O (x = 0, 0.01, 0.02, 0.03) and (UPu)O was measured with a dilatometer in an oxygen partial pressure-controlled atmosphere. The oxygen partial pressure was controlled to hold a constant oxygen-to-metal ratio in the (U,Pu)O during the measurement. Thermal expansion slightly increased with the decrease in oxygen-to-metal ratio. The relationship was derived to describe thermal expansion.

Improved holdup blender assay system (IBAS) slope validation measurements to improve nuclear material accountancy of high alpha holdup

LaFleur, A. M.*; Nakamura, Hironobu; Menlove, H. O.*; Mukai, Yasunobu; Swinhoe, M. T.*; Marlow, J. B.*; Kurita, Tsutomu

Proceedings of 37th ESARDA Annual Meeting (Internet), p.435 - 441, 2015/08

The IBAS (Improved Holdup Blender Assay System) system for safeguards and nuclear material accountancy (NMA) of holdup measurements is used at PCDF. The purpose of this detector is to measure the doubles rate from each glovebox in order to determine the mass of Pu holdup. In order to establish calibration curves for the IBAS detector and improve the holdup measurement methodology, JAEA conducted the IBAS calibration exercise with LANL support using MOX standards in 2010. In 2011, a cleanout exercise was performed and the results showed that the holdup removed from the glovebox had a significantly higher alpha term (alpha = 15.8 - 31.5) than the MOX standards (alpha = 0.67) used to establish the 2010 calibration curves. To further investigate these findings, JAEA conducted slope validation measurements in 2013 to confirm the validity of IBAS calibration slopes for the case of high alpha holdup. This paper describes the IBAS slope validation tests, analysis of the experimental results, and the evaluation of the need for a correction factor for the high alpha holdup. Quantifying the alpha term of the holdup in each glove box and understanding how this value changes over time is important to improving the overall NMA at PCDF. The results from this work will provide invaluable experimental data that directly supports safeguards and NMA measurements of plutonium holdup in gloveboxes.