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Title: Tricritical point from high-field magnetoelastic and metamagnetic effects in UN

Abstract

Uranium nitride (UN) is one of the most studied actinide materials as it is a promising fuel for the next generation of nuclear reactors. Despite large experimental and theoretical efforts, some of the fundamental questions such as degree of 5 f–electron localization/delocalization and its relationship to magneto-vibrational properties are not resolved yet. We show that the magnetostriction of UN measured in pulsed magnetic fields up to 65 T and below the Néel temperature is large and exhibits complex behavior with two transitions. While the high field anomaly is a field-induced metamagnetic-like transition and affects both magnetisation and magnetostriction, the low field anomaly does not contribute to the magnetic susceptibility. Our data suggest a change in the nature of the metamagnetic transition from first to second order-like at a tricritical point at T tri ~24 K and H tri ~52 T. The induced magnetic moment at 60 T might suggest that only one subset of magnetic moments has aligned along the field direction. Using the results obtained here we have constructed a magnetic phase diagram of UN. Our studies demonstrate that dilatometry in high fields is an effective method to investigate the magneto-structural coupling in actinide materials.

Authors:
 [1];  [1];  [2]; ORCiD logo [2];  [3];  [2];  [4];  [5];  [1]
  1. Idaho National Lab. (INL), Idaho Falls, ID (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. Idaho National Lab. (INL), Idaho Falls, ID (United States); Univ. of Nevada, Las Vegas, NV (United States). Dept. of Chemistry and Biochemistry, High Pressure Science and Engineering Center
  4. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Maria Curie-Sklodowska Univ., Lublin (Poland). Inst. of Physics
  5. European Commission, Karlsruhe (Germany). Joint Research Centre
Publication Date:
Research Org.:
Idaho National Lab. (INL), Idaho Falls, ID (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
OSTI Identifier:
1395024
Alternate Identifier(s):
OSTI ID: 1407862; OSTI ID: 1412856; OSTI ID: 1498253
Report Number(s):
LA-UR-17-30081; LA-UR-16-28832; INL/JOU-16-40525-Rev000
Journal ID: ISSN 2045-2322; PII: 6154
Grant/Contract Number:  
AC07-05ID14517; DMR-1157490; AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; electronic properties and materials; magnetic properties and materials; High Magnetic Field Science; 11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS; Uranium Nitride; Magnetostriction

Citation Formats

Shrestha, K., Antonio, D., Jaime, M., Harrison, N., Mast, D. S., Safarik, D., Durakiewicz, T., Griveau, J. -C., and Gofryk, K. Tricritical point from high-field magnetoelastic and metamagnetic effects in UN. United States: N. p., 2017. Web. doi:10.1038/s41598-017-06154-7.
Shrestha, K., Antonio, D., Jaime, M., Harrison, N., Mast, D. S., Safarik, D., Durakiewicz, T., Griveau, J. -C., & Gofryk, K. Tricritical point from high-field magnetoelastic and metamagnetic effects in UN. United States. doi:10.1038/s41598-017-06154-7.
Shrestha, K., Antonio, D., Jaime, M., Harrison, N., Mast, D. S., Safarik, D., Durakiewicz, T., Griveau, J. -C., and Gofryk, K. Wed . "Tricritical point from high-field magnetoelastic and metamagnetic effects in UN". United States. doi:10.1038/s41598-017-06154-7. https://www.osti.gov/servlets/purl/1395024.
@article{osti_1395024,
title = {Tricritical point from high-field magnetoelastic and metamagnetic effects in UN},
author = {Shrestha, K. and Antonio, D. and Jaime, M. and Harrison, N. and Mast, D. S. and Safarik, D. and Durakiewicz, T. and Griveau, J. -C. and Gofryk, K.},
abstractNote = {Uranium nitride (UN) is one of the most studied actinide materials as it is a promising fuel for the next generation of nuclear reactors. Despite large experimental and theoretical efforts, some of the fundamental questions such as degree of 5 f–electron localization/delocalization and its relationship to magneto-vibrational properties are not resolved yet. We show that the magnetostriction of UN measured in pulsed magnetic fields up to 65 T and below the Néel temperature is large and exhibits complex behavior with two transitions. While the high field anomaly is a field-induced metamagnetic-like transition and affects both magnetisation and magnetostriction, the low field anomaly does not contribute to the magnetic susceptibility. Our data suggest a change in the nature of the metamagnetic transition from first to second order-like at a tricritical point at T tri ~24 K and H tri ~52 T. The induced magnetic moment at 60 T might suggest that only one subset of magnetic moments has aligned along the field direction. Using the results obtained here we have constructed a magnetic phase diagram of UN. Our studies demonstrate that dilatometry in high fields is an effective method to investigate the magneto-structural coupling in actinide materials.},
doi = {10.1038/s41598-017-06154-7},
journal = {Scientific Reports},
number = 1,
volume = 7,
place = {United States},
year = {2017},
month = {7}
}

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Figures / Tables:

Figure 1 Figure 1: The temperature dependence of the heat capacity of UN (left hand scale) and the thermal expansion coefficient (−α) (right hand scale). A black arrow marks the Néel temperature at 52 K and red arrows mark anomalies in α described in the text. Lower inset: crystal structure of UN.more » Upper inset: magnetic structure of UN (see the text). Large green circles represent uranium atoms and small blue circles mark nitrogen atoms.« less

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.