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Title: $$\mathrm{^{239}Pu}$$ nuclear magnetic resonance in the candidate topological insulator $$\mathrm{PuB_4}$$

Abstract

In this article, we present a detailed nuclear magnetic resonance (NMR) study of $$\mathrm{^{239}Pu}$$ in bulk and powdered single-crystal plutonium tetraboride ($$\mathrm{PuB_4}$$), which has recently been investigated as a potential correlated topological insulator. This study constitutes the second-ever observation of the $$\mathrm{^{239}Pu}$$ NMR signal, and provides unique on-site sensitivity to the rich $$f$$-electron physics and insight into the bulk gaplike behavior in $$\mathrm{PuB_4}$$. The $$\mathrm{^{239}Pu}$$ NMR spectra are consistent with axial symmetry of the shift tensor showing for the first time that $$\mathrm{^{239}Pu}$$ NMR can be observed in an anisotropic environment and up to room temperature. The temperature dependence of the $$\mathrm{^{239}Pu}$$ shift, combined with a relatively long spin-lattice relaxation time ($$T_1$$), indicate that $$\mathrm{PuB_4}$$ adopts a nonmagnetic state with gaplike behavior consistent with our density functional theory calculations. The temperature dependencies of the NMR Knight shift and $$T_1^{1}$$ –microscopic quantities sensitive only to bulk states–imply bulk gaplike behavior confirming that $$\mathrm{PuB_4}$$ is a good candidate topological insulator. The large contrast between the $$\mathrm{^{239}Pu}$$ orbital shifts in the ionic insulator $$\mathrm{PuO_2} (\sim {+24.7 }\%)$$ and $$\mathrm{PuB_4} (\sim-0.5\%)$$ provides a new tool to investigate the nature of chemical bonding in plutonium materials.

Authors:
 [1];  [2];  [3];  [4];  [3];  [3];  [5];  [3];  [3];  [3];  [3];  [3]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Leibniz Institute for Solid State and Materials Research (IFW) Dresden (Germany)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Max Planck Inst. for Chemical Physics of Solids, Dresden (Germany)
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  4. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Japan Atomic Energy Agency, Tokai, Naka (Japan)
  5. Florida State Univ., Tallahassee, FL (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Actinide Science & Technology (CAST); Florida State Univ., Tallahassee, FL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1566685
Alternate Identifier(s):
OSTI ID: 1489316
Grant/Contract Number:  
SC0016568
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 99; Journal Issue: 3; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
73 NUCLEAR PHYSICS AND RADIATION PHYSICS; nuclear; defects; mechanical behavior; corrosion; charge transport; superconductivity; magnetism and spin physics; separations; geophysics/geochemistry; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); synthesis (predictive); synthesis (scalable processing)

Citation Formats

Dioguardi, A. P., Yasuoka, H., Thomas, S. M., Sakai, H., Cary, S. K., Kozimor, S. A., Albrecht-Schmitt, T. E., Choi, H. C., Zhu, J. -X., Thompson, J. D., Bauer, E. D., and Ronning, F. $\mathrm{^{239}Pu}$ nuclear magnetic resonance in the candidate topological insulator $\mathrm{PuB_4}$. United States: N. p., 2019. Web. doi:10.1103/physrevb.99.035104.
Dioguardi, A. P., Yasuoka, H., Thomas, S. M., Sakai, H., Cary, S. K., Kozimor, S. A., Albrecht-Schmitt, T. E., Choi, H. C., Zhu, J. -X., Thompson, J. D., Bauer, E. D., & Ronning, F. $\mathrm{^{239}Pu}$ nuclear magnetic resonance in the candidate topological insulator $\mathrm{PuB_4}$. United States. https://doi.org/10.1103/physrevb.99.035104
Dioguardi, A. P., Yasuoka, H., Thomas, S. M., Sakai, H., Cary, S. K., Kozimor, S. A., Albrecht-Schmitt, T. E., Choi, H. C., Zhu, J. -X., Thompson, J. D., Bauer, E. D., and Ronning, F. 2019. "$\mathrm{^{239}Pu}$ nuclear magnetic resonance in the candidate topological insulator $\mathrm{PuB_4}$". United States. https://doi.org/10.1103/physrevb.99.035104. https://www.osti.gov/servlets/purl/1566685.
@article{osti_1566685,
title = {$\mathrm{^{239}Pu}$ nuclear magnetic resonance in the candidate topological insulator $\mathrm{PuB_4}$},
author = {Dioguardi, A. P. and Yasuoka, H. and Thomas, S. M. and Sakai, H. and Cary, S. K. and Kozimor, S. A. and Albrecht-Schmitt, T. E. and Choi, H. C. and Zhu, J. -X. and Thompson, J. D. and Bauer, E. D. and Ronning, F.},
abstractNote = {In this article, we present a detailed nuclear magnetic resonance (NMR) study of $\mathrm{^{239}Pu}$ in bulk and powdered single-crystal plutonium tetraboride ($\mathrm{PuB_4}$), which has recently been investigated as a potential correlated topological insulator. This study constitutes the second-ever observation of the $\mathrm{^{239}Pu}$ NMR signal, and provides unique on-site sensitivity to the rich $f$-electron physics and insight into the bulk gaplike behavior in $\mathrm{PuB_4}$. The $\mathrm{^{239}Pu}$ NMR spectra are consistent with axial symmetry of the shift tensor showing for the first time that $\mathrm{^{239}Pu}$ NMR can be observed in an anisotropic environment and up to room temperature. The temperature dependence of the $\mathrm{^{239}Pu}$ shift, combined with a relatively long spin-lattice relaxation time ($T_1$), indicate that $\mathrm{PuB_4}$ adopts a nonmagnetic state with gaplike behavior consistent with our density functional theory calculations. The temperature dependencies of the NMR Knight shift and $T_1^{1}$ –microscopic quantities sensitive only to bulk states–imply bulk gaplike behavior confirming that $\mathrm{PuB_4}$ is a good candidate topological insulator. The large contrast between the $\mathrm{^{239}Pu}$ orbital shifts in the ionic insulator $\mathrm{PuO_2} (\sim {+24.7 }\%)$ and $\mathrm{PuB_4} (\sim-0.5\%)$ provides a new tool to investigate the nature of chemical bonding in plutonium materials.},
doi = {10.1103/physrevb.99.035104},
url = {https://www.osti.gov/biblio/1566685}, journal = {Physical Review B},
issn = {2469-9950},
number = 3,
volume = 99,
place = {United States},
year = {Wed Jan 02 00:00:00 EST 2019},
month = {Wed Jan 02 00:00:00 EST 2019}
}

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Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996


Absence of magnetic moments in plutonium
journal, August 2005


Topological insulators and superconductors
journal, October 2011


Fluctuating valence in a correlated solid and the anomalous properties of δ-plutonium
journal, March 2007


Sm B 6 : Kondo Insulator or Exotic Metal?
journal, February 1995


NMR Study of a Valence Fluctuating Compound SmB 6
journal, August 1981


Nuclear magnetic resonance in Kondo lattice systems
journal, May 2016


NMR Probe of Metallic States in Nanoscale Topological Insulators
journal, January 2013


Defect-induced magnetic fluctuations in YbB12
journal, June 2002


Surface Hall Effect and Nonlocal Transport in SmB6: Evidence for Surface Conduction
journal, November 2013


Self-irradiation damage to the local structure of plutonium and plutonium intermetallics
journal, March 2013


The valence-fluctuating ground state of plutonium
journal, July 2015


Plutonium Borides
journal, August 1965


Colloquium: Topological insulators
journal, November 2010


Interrelation between Dynamical and Static Spin Gaps in Quantum Spin Systems
journal, February 1997


Surface electronic structure of the topological Kondo-insulator candidate correlated electron system SmB6
journal, December 2013


The nuclear magnetic moment of plutonium-239
journal, September 1958


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


NMR nomenclature. Nuclear spin properties and conventions for chemical shifts(IUPAC Recommendations 2001)
journal, January 2001


Actinide Topological Insulator Materials with Strong Interaction
journal, March 2012


First-Principles Calculation of the Electric Field Gradient of Li 3 N
journal, March 1985


Observation of 239Pu Nuclear Magnetic Resonance
journal, May 2012


Solid state calculations using WIEN2k
journal, October 2003


SmB 6 : A Promising Candidate for a Topological Insulator
journal, December 2011


The crystal structure of some plutonium borides
journal, May 1960


The B-Pu (boron-plutonium) system
journal, September 1997


Plutonium-Based Heavy-Fermion Systems
journal, March 2015


Topological Kondo Insulators
journal, March 2016


171Yb NMR in the Kondo semiconductor YbB12
journal, June 2000


Recent Advances in Solid-State Nuclear Magnetic Resonance Spectroscopy
journal, June 2018


Valence fluctuations and quasiparticle multiplets in plutonium chalcogenides and pnictides
journal, January 2010


Site-selective electronic correlation in α-plutonium metal
journal, October 2013


Bi 209 NMR and NQR investigation of the small-gap semiconductor Ce 3 Bi 4 Pt 3
journal, June 1994


Principles of Magnetic Resonance
book, January 1990


First-order phase transition in UO 2 : 235 U and 17 O NMR study
journal, February 2001


Observation of possible topological in-gap surface states in the Kondo insulator SmB6 by photoemission
journal, December 2013


High-field suppression of in-gap states in the Kondo insulator Sm B 6
journal, February 2007