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Title: The valence-fluctuating ground state of plutonium

Journal Article · · Science Advances
 [1];  [1];  [2];  [3];  [3];  [1];  [1];  [4];  [1];  [1];  [1];  [1];  [1];  [2];  [2];  [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Rutgers Univ., Piscataway, NJ (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Institute for Transuranium Elements, Karlsruhe (Germany)

A central issue in material science is to obtain understanding of the electronic correlations that control complex materials. Such electronic correlations frequently arise because of the competition of localized and itinerant electronic degrees of freedom. Although the respective limits of well-localized or entirely itinerant ground states are well understood, the intermediate regime that controls the functional properties of complex materials continues to challenge theoretical understanding. We have used neutron spectroscopy to investigate plutonium, which is a prototypical material at the brink between bonding and nonbonding configurations. In addition, our study reveals that the ground state of plutonium is governed by valence fluctuations, that is, a quantum mechanical superposition of localized and itinerant electronic configurations as recently predicted by dynamical mean field theory. Our results not only resolve the long-standing controversy between experiment and theory on plutonium’s magnetism but also suggest an improved understanding of the effects of such electronic dichotomy in complex materials.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
AC52-06NA25396
OSTI ID:
1236683
Report Number(s):
LA-UR-15-20256
Journal Information:
Science Advances, Vol. 1, Issue 6; ISSN 2375-2548
Publisher:
AAASCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 78 works
Citation information provided by
Web of Science

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Cited By (20)

Pressure-driven 5 f localized-itinerant transition and valence fluctuation in cubic phase californium journal January 2019
Phonon and magnetic structure in δ-plutonium from density-functional theory journal October 2015
Valence fluctuation for f electrons in XGaO3 (X = Pu, Ce): a perspective from dynamic mean field theory journal October 2019
Lattice dynamics and elasticity for ε-plutonium journal April 2017
Electronic correlations in cerium’s high-pressure phases journal September 2018
Origin of the multiple configurations that drive the response of δ-plutonium’s elastic moduli to temperature journal September 2016
Characterization of berkelium(III) dipicolinate and borate compounds in solution and the solid state journal August 2016
A unified and efficient theory for the structural properties of actinides and phases of plutonium journal September 2018
Thermodynamics of the bulk modulus of delta phase plutonium alloys journal March 2019
Instability of the f -electron state in URu 2 Si 2 − x P x probed using high magnetic fields journal June 2019
Magnetic order and valence fluctuation in a PuGa intermetallic compound studied via a first principles calculation journal November 2019
Oxidation states and ionicity journal October 2018
Toward a predictive theory of correlated materials journal July 2018
Phase stabilization by electronic entropy in plutonium journal July 2019
Density-functional theory for plutonium journal January 2019
Site and orbital selective correlations in $β$-Pu text January 2018
Isochronal annealing effects on local structure, crystalline fraction, and undamaged region size of radiation damage in Ga-stabilized δ -Pu journal July 2016
Observation of 5f intermediate coupling in uranium x-ray emission spectroscopy journal January 2020
Anomalous thermodynamic properties and phase stability of δ Pu 1 x M x ( M = Ga and Al ) alloys from first-principles calculations journal December 2016
Electronic and vibrational properties of Pu 3 M ( M = Al ,   Ga ,   In ,   and   Tl ) : A first-principles study journal November 2019

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