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Title: Pseudogap in elemental plutonium

Abstract

Electronic correlations associated with incipient magnetism have long been recognized as an important factor in stabilizing the largest atomic volume δ phase of plutonium, although their strength compared to those in the rare earths and neighboring actinides in the periodic table has largely remained a mystery. We show here using calorimetry measurements, together with prior detailed measurements of the phonon dispersion, that the 5f electrons of the δ phase reside in a pseudogapped state, accompanied by reductions in various physical properties below a characteristic temperature T* ≈ 100 K. The small characteristic energy scale of the pseudogapped state implies that the 5f electrons in plutonium are much closer to the threshold for localization and magnetic order than has been suggested by state-of-the-art electronic structure theory, revealing plutonium to be arguably the most strongly correlated of the elements.

Authors:
 [1];  [1]; ORCiD logo [1]; ORCiD logo [1];  [1];  [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Univ. of Florida, Gainesville, FL (United States). National High Magnetic Field Lab. (MagLab)
Sponsoring Org.:
USDOE Office of Science (SC); USDOE Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF)
OSTI Identifier:
1874164
Report Number(s):
LA-UR-20-24656
Journal ID: ISSN 2469-9950; TRN: US2306644
Grant/Contract Number:  
89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review. B
Additional Journal Information:
Journal Volume: 105; Journal Issue: 4; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; density of states; electronic structure; Kondo effect; transport phenomena; magnetism; magnetic susceptibility

Citation Formats

Wartenbe, Mark, Tobash, Paul H., Singleton, John, Winter Stritzinger, Laurel Elaine, Richmond, Scott, and Harrison, Neil. Pseudogap in elemental plutonium. United States: N. p., 2022. Web. doi:10.1103/physrevb.105.l041107.
Wartenbe, Mark, Tobash, Paul H., Singleton, John, Winter Stritzinger, Laurel Elaine, Richmond, Scott, & Harrison, Neil. Pseudogap in elemental plutonium. United States. https://doi.org/10.1103/physrevb.105.l041107
Wartenbe, Mark, Tobash, Paul H., Singleton, John, Winter Stritzinger, Laurel Elaine, Richmond, Scott, and Harrison, Neil. Thu . "Pseudogap in elemental plutonium". United States. https://doi.org/10.1103/physrevb.105.l041107. https://www.osti.gov/servlets/purl/1874164.
@article{osti_1874164,
title = {Pseudogap in elemental plutonium},
author = {Wartenbe, Mark and Tobash, Paul H. and Singleton, John and Winter Stritzinger, Laurel Elaine and Richmond, Scott and Harrison, Neil},
abstractNote = {Electronic correlations associated with incipient magnetism have long been recognized as an important factor in stabilizing the largest atomic volume δ phase of plutonium, although their strength compared to those in the rare earths and neighboring actinides in the periodic table has largely remained a mystery. We show here using calorimetry measurements, together with prior detailed measurements of the phonon dispersion, that the 5f electrons of the δ phase reside in a pseudogapped state, accompanied by reductions in various physical properties below a characteristic temperature T* ≈ 100 K. The small characteristic energy scale of the pseudogapped state implies that the 5f electrons in plutonium are much closer to the threshold for localization and magnetic order than has been suggested by state-of-the-art electronic structure theory, revealing plutonium to be arguably the most strongly correlated of the elements.},
doi = {10.1103/physrevb.105.l041107},
journal = {Physical Review. B},
number = 4,
volume = 105,
place = {United States},
year = {Thu Jan 13 00:00:00 EST 2022},
month = {Thu Jan 13 00:00:00 EST 2022}
}

Works referenced in this record:

Freezing out of a low-energy bulk spin exciton in SmB6
journal, August 2018


Ordering of the Face-Centered-Cubic Lattice with Nearest-Neighbor Interaction
journal, September 1980


Equilibrium properties of delta-Pu: LDA+ U calculations (LDAequiv local density approximation)
journal, February 2000


Heat capacity, thermal expansion and electrical resistivity of an 8 a/o aluminum-plutonium (delta-phase stabilized) alloy below 300°K
journal, November 1960


Spin susceptibility of Ga-stabilized δ Pu probed by Ga 69 NMR
journal, May 2005


Pu Electronic Structure and Photoelectron Spectroscopy
journal, January 2011


Self-interaction-corrected local spin density theory of 5 f electron localization in actinides
journal, September 2007


4 f Crystal Field Ground State of the Strongly Correlated Topological Insulator SmB 6
journal, January 2018


Electronic properties of f -electron metals using the generalized gradient approximation
journal, September 1994


Three-dimensional resonating-valence-bond liquids and their excitations
journal, November 2003


Plutonium-based superconductivity with a transition temperature above 18 K
journal, November 2002

  • Sarrao, J. L.; Morales, L. A.; Thompson, J. D.
  • Nature, Vol. 420, Issue 6913
  • DOI: 10.1038/nature01212

Specific Heat of δ -Pu Stabilized by Am
journal, April 2006


Multiconfigurational nature of 5f orbitals in uranium and plutonium intermetallics
journal, June 2012

  • Booth, C. H.; Jiang, Y.; Wang, D. L.
  • Proceedings of the National Academy of Sciences, Vol. 109, Issue 26
  • DOI: 10.1073/pnas.1200725109

Fermi arcs in a doped pseudospin-1/2 Heisenberg antiferromagnet
journal, June 2014


Correlated electrons in δ-plutonium within a dynamical mean-field picture
journal, April 2001

  • Savrasov, S. Y.; Kotliar, G.; Abrahams, E.
  • Nature, Vol. 410, Issue 6830
  • DOI: 10.1038/35071035

Observation of a d-wave gap in electron-doped Sr2IrO4
journal, October 2015

  • Kim, Y. K.; Sung, N. H.; Denlinger, J. D.
  • Nature Physics, Vol. 12, Issue 1
  • DOI: 10.1038/nphys3503

Density-functional investigation of magnetism in δ -Pu
journal, November 2002


Phase stability and phase transformations in Pu–Ga alloys
journal, January 2004


Hall Effect in Plutonium
journal, March 1965


Gallium stabilization of δ Pu : Density-functional calculations
journal, November 2005


Resistivite electrique des solutions solides d'alliages Pu-Ga en phase δ a tres basses temperatures (4,2–300° K)
journal, September 1971


Absence of magnetic moments in plutonium
journal, August 2005


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


Coulomb- U and magnetic-moment collapse in δ-Pu
journal, February 2005


Density-functional theory for plutonium
journal, January 2019


Phonon Dispersions of fcc  -Plutonium-Gallium by Inelastic X-ray Scattering
journal, August 2003


69Ga NMR and magnetic susceptibility in δ-phase of Pu1−xGax (x=0.05, x=0.08) alloys
journal, March 2009


Spectral properties of δ -plutonium: Sensitivity to 5 f occupancy
journal, December 2007


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

  • Janoschek, Marc; Das, Pinaki; Chakrabarti, Bismayan
  • Science Advances, Vol. 1, Issue 6
  • DOI: 10.1126/sciadv.1500188

Phase stabilization by electronic entropy in plutonium
journal, July 2019


Introduction to Many-Body Physics
book, December 2015


Quantum Mechanics: The Key to Understanding Magnetism
journal, July 1978


Nature of the 5 f states in actinide metals
journal, February 2009


Experimental Electronic Heat Capacities of α - and δ -Plutonium: Heavy-Fermion Physics in an Element
journal, November 2003


The pseudogap in high-temperature superconductors: an experimental survey
journal, January 1999


A novel electronic configuration of the 5f states in δ-plutonium as revealed by the photo-electron spectra
journal, April 2004

  • Wills, J. M.; Eriksson, O.; Delin, A.
  • Journal of Electron Spectroscopy and Related Phenomena, Vol. 135, Issue 2-3
  • DOI: 10.1016/j.elspec.2004.02.169

Unusual Phonon Softening in δ -Phase Plutonium
journal, April 2004


Localization of 5f electrons in δ-plutonium: Evidence for the Kondo effect
journal, January 1996


Correlation between Bulk Thermodynamic Measurements and the Low-Temperature-Resistance Plateau in SmB 6
journal, July 2014


Heavy fermion semiconductors
journal, May 2000


Electronic correlation induced expansion of Fermi pockets in δ -plutonium
journal, June 2020


Origin of the multiple configurations that drive the response of δ-plutonium’s elastic moduli to temperature
journal, September 2016

  • Migliori, Albert; Söderlind, Per; Landa, Alexander
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 40
  • DOI: 10.1073/pnas.1609215113

Metal-Insulator Transition
journal, October 1968


Kondo universality, energy scales, and intermediate valence in plutonium
journal, July 2009

  • Clementyev, E. S.; Mirmelstein, A. V.
  • Journal of Experimental and Theoretical Physics, Vol. 109, Issue 1
  • DOI: 10.1134/S1063776109070164

Doping a Mott insulator: Physics of high-temperature superconductivity
journal, January 2006

  • Lee, Patrick A.; Nagaosa, Naoto; Wen, Xiao-Gang
  • Reviews of Modern Physics, Vol. 78, Issue 1
  • DOI: 10.1103/RevModPhys.78.17

Novel electronic configuration in ∂−Pu
journal, June 1999


Lecture Notes on Electron Correlation and Magnetism
book, January 1999


Reply to Janoschek et al.: The excited δ-phase of plutonium
journal, January 2017

  • Migliori, Albert; Söderlind, Per; Landa, Alexander
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 3
  • DOI: 10.1073/pnas.1619207114

Emergent magnetic moments produced by self-damage in plutonium
journal, November 2006

  • McCall, S. K.; Fluss, M. J.; Chung, B. W.
  • Proceedings of the National Academy of Sciences, Vol. 103, Issue 46
  • DOI: 10.1073/pnas.0608552103

Relevance of Kondo physics for the temperature dependence of the bulk modulus in plutonium
journal, January 2017

  • Janoschek, Marc; Lander, Gerry; Lawrence, Jon M.
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 3
  • DOI: 10.1073/pnas.1618967114

Invar model for δ-phase Pu: thermal expansion, elastic and magnetic properties
journal, June 2006