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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. Here 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. These 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]
+ Show Author Affiliations
  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 Laboratory (INL), Idaho Falls, ID (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); 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.
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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. https://doi.org/10.1038/s41598-017-06154-7
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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. https://doi.org/10.1038/s41598-017-06154-7. https://www.osti.gov/servlets/purl/1395024.
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@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. Here 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. These 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 = {Wed Jul 26 00:00:00 EDT 2017},
month = {Wed Jul 26 00:00:00 EDT 2017}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/s41598-017-06154-7
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Cited by: 19 works
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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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Works referenced in this record:

Magnetic anisotropy in the frustrated spin-chain compound β − TeVO 4
journal, August 2016

Uranium azide photolysis results in C–H bond activation and provides evidence for a terminal uranium nitride
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High resolution magnetostriction measurements in pulsed magnetic fields using fiber Bragg gratings
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  • Review of Scientific Instruments, Vol. 81, Issue 3
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Thermal-expansion and magnetostriction study on UNiAl single crystals
journal, January 2002

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Magnetostriction and magnetic texture to 100.75 Tesla in frustrated SrCu2(BO3)2
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journal, October 1980

Magnetic susceptibility of the uranium nitrides
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High-resolution angle-resolved photoemission study of UN and USb; Dual character of 5f electrons
journal, May 2001

Electronic structure of UN based on specific heat and field-induced transitions up to 65 T
journal, December 2016

The Structures of the Carbides, Nitrides and Oxides of Uranium 1
journal, January 1948

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Thermal expansion and crystal structure of FeSi between 4 and 1173 K determined by time-of-flight neutron powder diffraction
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Magnetic properties of uranium monopnictides
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Equation of State in the Neighborhood of the Critical Point
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Metamagnetism
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Itinerant nature of U 5 f states in uranium mononitride revealed by angle-resolved photoelectron spectroscopy
journal, December 2012

Magnetic properties of single-crystal uranium mononitride
journal, August 1977

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Tricritical point of the f -electron antiferromagnet US b 2 driven by high magnetic fields
journal, January 2017

Magnetic susceptibility, electrical resistivity and elastic constants of antiferromagnetic un single crystals
journal, January 1977

Electronic structure and magnetic and transport properties of single-crystalline UN
journal, October 2007

Magnetization of uranium monopnictides in fields up to 40 T
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The high-pressure effect of an electronic state in uranium compounds: UPtGa 5 and UN
journal, July 2003

Uranium Mononitride: Heat Capacity and Thermodynamic Properties from 5° to 350°K
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Negative thermal expansion and antiferromagnetism in the actinide oxypnictide NpFeAsO
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Critical Behavior Near the Paramagnetic to Ferromagnetic Phase Transition Temperature in Sr1.5Nd0.5MnO4 Compound
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Degree of the Critical Isotherm
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Negative thermal expansion and antiferromagnetism in the actinide oxypnictide NpFeAsO
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Thermal expansion and crystal structure of FeSi between 4 and 1173 K determined by time-of-flight neutron powder diffraction
journal, March 2002

  • Vočadlo, L.; Knight, K. S.; Price, G. D.
  • Physics and Chemistry of Minerals, Vol. 29, Issue 2
  • DOI: 10.1007/s002690100202

Magnetization of uranium monopnictides in fields up to 40 T
journal, December 1978

The Structures of the Carbides, Nitrides and Oxides of Uranium 1
journal, January 1948

  • Rundle, R. E.; Baenziger, N. C.; Wilson, A. S.
  • Journal of the American Chemical Society, Vol. 70, Issue 1
  • DOI: 10.1021/ja01181a029

Uranium azide photolysis results in C–H bond activation and provides evidence for a terminal uranium nitride
journal, July 2010

  • Thomson, Robert K.; Cantat, Thibault; Scott, Brian L.
  • Nature Chemistry, Vol. 2, Issue 9
  • DOI: 10.1038/nchem.705

Equation of State in the Neighborhood of the Critical Point
journal, December 1965

  • Widom, B.
  • The Journal of Chemical Physics, Vol. 43, Issue 11
  • DOI: 10.1063/1.1696618

High resolution magnetostriction measurements in pulsed magnetic fields using fiber Bragg gratings
journal, March 2010

  • Daou, Ramzy; Weickert, Franziska; Nicklas, Michael
  • Review of Scientific Instruments, Vol. 81, Issue 3
  • DOI: 10.1063/1.3356980

Metamagnetism
journal, September 1977

Magnetic Susceptibility of UC 1- x N x from 4° to 1,100°K
journal, January 1972

  • Ohmichi, Toshihiko; Nasu, Shoichi; Kikuchi, Takeo
  • Journal of Nuclear Science and Technology, Vol. 9, Issue 1
  • DOI: 10.1080/18811248.1972.9734790

An investigation of the magnetic structure of uranium nitride by neutron diffraction
journal, December 1965

Nature of the 5 f electrons in uranium nitride: A photoelectron spectroscopic study of UN, U, U O 2 , ThN, and Th
journal, March 1980

Itinerant- 5 f -electron antiferromagnetism in uranium nitride: A temperature-dependent angle-resolved photoemission study
journal, August 1983

The crystal structure of UN by neutron diffraction
journal, October 1958

Critical Scaling of the Magnetization and Magnetostriction in the Weak Itinerant Ferromagnet UIr
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    Works referencing / citing this record:

    Lewis acid capping of a uranium( v ) nitride via a uranium( iii ) azide molecular square
    journal, January 2020

    • Boreen, Michael A.; Rao, Guodong; Villarreal, David G.
    • Chemical Communications, Vol. 56, Issue 33
    • DOI: 10.1039/d0cc01356k

    Magnetotransport as a probe of phase transformations in metallic antiferromagnets: The case of UIrS i 3
    journal, July 2019

    Fiber Bragg Grating Dilatometry in Extreme Magnetic Field and Cryogenic Conditions
    journal, November 2017

    • Jaime, Marcelo; Corvalán Moya, Carolina; Weickert, Franziska
    • Sensors, Vol. 17, Issue 11
    • DOI: 10.3390/s17112572
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