Structural differences between single crystal and polycrystalline UBe13

Volz, Heather Michelle; Vogel, Sven C.; Smith, Alice Iulia; Smith, James L.; Fisk, Zachary; Winkler, Bjorn; Dirmyer, Matthew R.; Judge, Elizabeth

doi:10.1080/14786435.2018.1468578

Title: Structural differences between single crystal and polycrystalline UBe₁₃

Abstract

Here, we report on observations of structural and chemical differences between samples of UBe₁₃ that were synthesised using two different methods. Unexplained discrepancies in properties between samples with differing synthesis had previously been found in this heavy fermion superconductor. A polycrystalline UBe₁₃ sample was made by arc-melting the constituents. Single crystals were grown using an aluminium flux and had a consistently slightly larger lattice parameter than the polycrystals, which merited further study. Neutron diffraction data were collected at the Lujan Center at LANSCE on the HIPPO diffractometer. Aluminium was detected by inductively coupled plasma mass spectrometry (ICP-MS) in the flux-grown single crystal (0.803 wt%), and small amounts (~0.2 wt%) of thorium were detected in the UBe₁₃ polycrystalline sample. In order to probe the implications of the presence of Al, calculations by spin-polarised DFT-GGA+U show that the incorporation of Al onto the 96i site (the lowest symmetry site in the structure) is energetically more favourable than on other sites. In general, the trends calculated by DFT for bond lengths and lattice parameter increases are consistent with bond lengths experimentally observed by neutron diffraction, but specific percentage changes with aluminium incorporation may be obscured by the unexpected thorium in the polycrystalline sample.more »« less

Authors:

Volz, Heather Michelle ^[1];

^[1];

^[1]; Smith, James L. ^[1]; Fisk, Zachary ^[2]; Winkler, Bjorn ^[3]; Dirmyer, Matthew R. ^[1];

^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Univ. of California, Irvine, CA (United States)
Goethe Univ., Frankfurt (Germany)

Publication Date:: Wed May 16 00:00:00 EDT 2018

Research Org.:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1440472

Report Number(s):: LA-UR-17-21717
Journal ID: ISSN 1478-6435

Grant/Contract Number:: AC52-06NA25396

Resource Type:: Accepted Manuscript

Journal Name:: Philosophical Magazine (2003, Print)

Additional Journal Information:: Journal Name: Philosophical Magazine (2003, Print); Journal Volume: 98; Journal Issue: 22; Journal ID: ISSN 1478-6435

Publisher:: Taylor & Francis

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; Heavy fermion; synthesis; impurities; crystal; neutron diffraction

Citation Formats


                    Volz, Heather Michelle, Vogel, Sven C., Smith, Alice Iulia, Smith, James L., Fisk, Zachary, Winkler, Bjorn, Dirmyer, Matthew R., and Judge, Elizabeth. Structural differences between single crystal and polycrystalline UBe13.  United States: N. p., 2018. 
Web.  doi:10.1080/14786435.2018.1468578.

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                    Volz, Heather Michelle, Vogel, Sven C., Smith, Alice Iulia, Smith, James L., Fisk, Zachary, Winkler, Bjorn, Dirmyer, Matthew R., & Judge, Elizabeth. Structural differences between single crystal and polycrystalline UBe13.  United States.  https://doi.org/10.1080/14786435.2018.1468578

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                    Volz, Heather Michelle, Vogel, Sven C., Smith, Alice Iulia, Smith, James L., Fisk, Zachary, Winkler, Bjorn, Dirmyer, Matthew R., and Judge, Elizabeth. Wed .  
"Structural differences between single crystal and polycrystalline UBe13".  United States.  https://doi.org/10.1080/14786435.2018.1468578.  https://www.osti.gov/servlets/purl/1440472.

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@article{osti_1440472,

  title        = {Structural differences between single crystal and polycrystalline UBe13},

  author       = {Volz, Heather Michelle and Vogel, Sven C. and Smith, Alice Iulia and Smith, James L. and Fisk, Zachary and Winkler, Bjorn and Dirmyer, Matthew R. and Judge, Elizabeth},

  abstractNote = {Here, we report on observations of structural and chemical differences between samples of UBe13 that were synthesised using two different methods. Unexplained discrepancies in properties between samples with differing synthesis had previously been found in this heavy fermion superconductor. A polycrystalline UBe13 sample was made by arc-melting the constituents. Single crystals were grown using an aluminium flux and had a consistently slightly larger lattice parameter than the polycrystals, which merited further study. Neutron diffraction data were collected at the Lujan Center at LANSCE on the HIPPO diffractometer. Aluminium was detected by inductively coupled plasma mass spectrometry (ICP-MS) in the flux-grown single crystal (0.803 wt%), and small amounts (~0.2 wt%) of thorium were detected in the UBe13 polycrystalline sample. In order to probe the implications of the presence of Al, calculations by spin-polarised DFT-GGA+U show that the incorporation of Al onto the 96i site (the lowest symmetry site in the structure) is energetically more favourable than on other sites. In general, the trends calculated by DFT for bond lengths and lattice parameter increases are consistent with bond lengths experimentally observed by neutron diffraction, but specific percentage changes with aluminium incorporation may be obscured by the unexpected thorium in the polycrystalline sample. The aggregate of our initial observations suggests that incorporation of aluminium from the flux into single crystal UBe13 is significant.},

  doi          = {10.1080/14786435.2018.1468578},

  journal      = {Philosophical Magazine (2003, Print)},

  number       = 22,

  volume       = 98,

  place        = {United States},

  year         = {Wed May 16 00:00:00 EDT 2018},

  month        = {Wed May 16 00:00:00 EDT 2018}

}

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https://doi.org/10.1080/14786435.2018.1468578

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Figure 1: U-Be binary phase diagram.

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Works referenced in this record:

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Works referencing / citing this record:

UBe13 and U1−xThxBe13: Unconventional Superconductors
journal, January 2019

Stewart, G. R.
Journal of Low Temperature Physics, Vol. 195, Issue 1-2
DOI: 10.1007/s10909-018-02140-z

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Title: Structural differences between single crystal and polycrystalline UBe13

Abstract

Citation Formats

Figures / Tables:

gsaslanguage: a GSAS script language for automated Rietveld refinements of diffraction data journal, July 2011

Generalized Gradient Approximation Made Simple journal, October 1996

Study of heavy-fermion compounds under high pressure journal, January 1987

U Be 13 : An Unconventional Actinide Superconductor journal, May 1983

Influence of impurities and magnetic fields on the normal and superconducting states of UBe 13 journal, January 1986

Signature of superconductivity in U Be 13 as seen by neutron scattering: Superconducting and magnetic energy scales journal, June 2014

Beryllium’s monocrystal and polycrystal elastic constants journal, March 2004

Special points for Brillouin-zone integrations journal, June 1976

Superconducting phases of f -electron compounds journal, November 2009

Observation of an Unusual Magnetic Anomaly in the Superconducting Mixed State of Heavy-Fermion Compound UBe 13 by Precise dc Magnetization Measurements journal, November 2012

Texture measurements using the new neutron diffractometer HIPPO and their analysis using the Rietveld method journal, March 2004

Elasticity of hexagonal BeO journal, December 2000

VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data journal, October 2011

Chemical physics of heavy electron uranium compounds journal, June 1987

Heavy-electron metals journal, March 1986

Beryllium-uranium system journal, February 1953

Field-Orientation Dependence of Low-Energy Quasiparticle Excitations in the Heavy-Electron Superconductor UBe 13 journal, April 2015

Measurement of acoustic phonons in UBe 13 journal, May 1986

First principles methods using CASTEP journal, January 2005

Impurities in the heavy‐fermion superconductor UBe 1 3 (invited) journal, March 1984

Interplay between superconductivity and magnetism journal, October 1995

Spin gap in heavy fermion compound UBe 13 journal, August 2016

Texture analysis with the new HIPPO TOF diffractometer journal, December 2003

Lattice parameter and hardness measurements on high purity beryllium journal, March 1963

Absolute Präzisionsbestimmung von Gitterkonstanten an Germanium- und Aluminium-Einkristallen mit Elektroneninterferenzen journal, January 1967

UBe13 and U1−xThxBe13: Unconventional Superconductors journal, January 2019

Title: Structural differences between single crystal and polycrystalline UBe₁₃

gsaslanguage: a GSAS script language for automated Rietveld refinements of diffraction data
journal, July 2011

Generalized Gradient Approximation Made Simple
journal, October 1996

Study of heavy-fermion compounds under high pressure
journal, January 1987

U ${Be}_{13}$ : An Unconventional Actinide Superconductor
journal, May 1983

Influence of impurities and magnetic fields on the normal and superconducting states of ${UBe}_{13}$
journal, January 1986

Signature of superconductivity in $U {Be}_{13}$ as seen by neutron scattering: Superconducting and magnetic energy scales
journal, June 2014

Beryllium’s monocrystal and polycrystal elastic constants
journal, March 2004

Special points for Brillouin-zone integrations
journal, June 1976

Superconducting phases of $f$ -electron compounds
journal, November 2009

Observation of an Unusual Magnetic Anomaly in the Superconducting Mixed State of Heavy-Fermion Compound ${UBe}_{13}$ by Precise dc Magnetization Measurements
journal, November 2012

Texture measurements using the new neutron diffractometer HIPPO and their analysis using the Rietveld method
journal, March 2004

Elasticity of hexagonal BeO
journal, December 2000

VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data
journal, October 2011

Chemical physics of heavy electron uranium compounds
journal, June 1987

Heavy-electron metals
journal, March 1986

Beryllium-uranium system
journal, February 1953

Field-Orientation Dependence of Low-Energy Quasiparticle Excitations in the Heavy-Electron Superconductor ${UBe}_{13}$
journal, April 2015

Measurement of acoustic phonons in ${UBe}_{13}$
journal, May 1986

First principles methods using CASTEP
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Impurities in the heavy‐fermion superconductor UBe ₁ ₃ (invited)
journal, March 1984

Interplay between superconductivity and magnetism
journal, October 1995

Spin gap in heavy fermion compound UBe ₁₃
journal, August 2016

Texture analysis with the new HIPPO TOF diffractometer
journal, December 2003

Lattice parameter and hardness measurements on high purity beryllium
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journal, January 1967

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journal, January 2019