skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Correlation strength and orbital differentiation across the phase diagram of plutonium metal

Abstract

We compare the trends on the strength of electronic correlations across the different phases of elemental Pu focusing on its site and orbital dependence, using a combination of density functional theory (DFT) and dynamical mean-field theory (DMFT) calculations within the vertex corrected one crossing approximation. We find that Pu-5f states are more correlated in δ -Pu, followed by some crystallographic sites in α and β phases. In addition, we observe that Pu-5f 5/2 and Pu-5f 7/2 orbital differentiation is a general feature of this material, as is site differentiation in the low-symmetry phases. The Pu-5f 5/2 states show Fermi liquid like behavior, whereas the Pu-5f 7/2 states remaining incoherent down to very low temperatures. We correlate the correlation strength in the different phases to their structure and the Pu-5 f occupancy of their crystallographic sites.

Authors:
ORCiD logo [1];  [2]
  1. Univ. Federal de Minas Gerais, Belo Horizonte, MG (Brazil); Rutgers Univ., Piscataway, NJ (United States)
  2. Rutgers Univ., Piscataway, NJ (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1760642
Report Number(s):
BNL-220813-2021-JAAM
Journal ID: ISSN 2469-9950
Grant/Contract Number:  
SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 102; Journal Issue: 24; 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; Electronic structure; First-principles calculations; Strongly correlated systems; Dynamical mean field theory

Citation Formats

Brito, W. H., and Kotliar, G. Correlation strength and orbital differentiation across the phase diagram of plutonium metal. United States: N. p., 2020. Web. doi:10.1103/physrevb.102.245111.
Brito, W. H., & Kotliar, G. Correlation strength and orbital differentiation across the phase diagram of plutonium metal. United States. https://doi.org/10.1103/physrevb.102.245111
Brito, W. H., and Kotliar, G. Tue . "Correlation strength and orbital differentiation across the phase diagram of plutonium metal". United States. https://doi.org/10.1103/physrevb.102.245111.
@article{osti_1760642,
title = {Correlation strength and orbital differentiation across the phase diagram of plutonium metal},
author = {Brito, W. H. and Kotliar, G.},
abstractNote = {We compare the trends on the strength of electronic correlations across the different phases of elemental Pu focusing on its site and orbital dependence, using a combination of density functional theory (DFT) and dynamical mean-field theory (DMFT) calculations within the vertex corrected one crossing approximation. We find that Pu-5f states are more correlated in δ -Pu, followed by some crystallographic sites in α and β phases. In addition, we observe that Pu-5f5/2 and Pu-5f 7/2 orbital differentiation is a general feature of this material, as is site differentiation in the low-symmetry phases. The Pu-5f5/2 states show Fermi liquid like behavior, whereas the Pu-5f7/2 states remaining incoherent down to very low temperatures. We correlate the correlation strength in the different phases to their structure and the Pu-5 f occupancy of their crystallographic sites.},
doi = {10.1103/physrevb.102.245111},
url = {https://www.osti.gov/biblio/1760642}, journal = {Physical Review B},
issn = {2469-9950},
number = 24,
volume = 102,
place = {United States},
year = {2020},
month = {12}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on December 8, 2021
Publisher's Version of Record

Save / Share:

Works referenced in this record:

Limits for ordered magnetism in Pu from muon spin rotation spectroscopy
journal, March 2006


Generalized Gradient Approximation Made Simple
journal, October 1996


Lattice dynamics and elasticity for ε-plutonium
journal, April 2017


The Anderson model with finite Coulomb repulsion
journal, December 1989


Racah materials: role of atomic multiplets in intermediate valence systems
journal, October 2015


Nature of the 5 f electronic structure of plutonium
journal, March 2020


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


The ab initio ground state properties and magnetic structure of plutonium
journal, April 2003


The crystal structure of beta plutonium metal
journal, May 1963


Janus-Faced Influence of Hund’s Rule Coupling in Strongly Correlated Materials
journal, December 2011


First-principles calculations of the electronic structure and spectra of strongly correlated systems: the LDA + U method
journal, January 1997


Electronic properties of Pu 19 Os simulating β-Pu: the strongly correlated Pu phase
journal, February 2018


Site and orbital selective correlations in β -Pu
journal, March 2019


Competition between delocalization and spin-orbit splitting in the actinide 5 f states
journal, August 2005


Sommerfeld coefficient of δ -Pu determined via a low-temperature specific heat Pu-Ce study
journal, October 2010


Many-Body Electronic Structure of Americium Metal
journal, January 2006


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


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


Phonon and magnetic structure in δ-plutonium from density-functional theory
journal, October 2015


A unified and efficient theory for the structural properties of actinides and phases of plutonium
journal, September 2018


Orbital differentiation in Hund metals
journal, September 2019


X-ray absorption branching ratio in actinides: LDA+DMFT approach
journal, January 2009


Density-Functional Calculations of α , β , γ , δ , δ , and ϵ Plutonium
journal, May 2004


µSR Studies of Pu Metal and the Pu-based Superconductor PuCoGa 5
journal, January 2006


Multiplet structure in Pu-based compounds: A photoemission case study of PuSi x ( 0.5 x 2 ) films
journal, April 2005


Effective Coulomb interaction in actinides from linear response approach
journal, January 2020


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


Orbital-Selective Mott Transitions in the Degenerate Hubbard Model
journal, May 2004


Orbital-dependent correlations in PuCoGa 5
journal, July 2018


Ground State Theory of δ Pu
journal, April 2000


Orbital selectivity in Hund's metals: The iron chalcogenides
journal, January 2013


Density-functional theory for plutonium
journal, January 2019


Elastic properties of Pu metal and Pu-Ga alloys
journal, June 2010


Assessing Relativistic Effects and Electron Correlation in the Actinide Metals Th to Pu
journal, November 2019


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


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


Kinetic frustration and the nature of the magnetic and paramagnetic states in iron pnictides and iron chalcogenides
journal, September 2011


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


Phase Diagram and Electronic Structure of Praseodymium and Plutonium
journal, January 2015


Hund’s coupling and its key role in tuning multiorbital correlations
journal, May 2011


Unified character of correlation effects in unconventional Pu-based superconductors and δ -Pu
journal, January 2013


Electronic Coherence in δ -Pu: A Dynamical Mean-Field Theory Study
journal, August 2008


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


Geometry and electronic structure of α -Pu: A theoretical study
journal, December 2003


Electronic structure and correlation effects in PuCoIn 5 as compared to PuCoGa 5
journal, February 2012


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


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


Oxidation and aging in U and Pu probed by spin-orbit sum rule analysis: Indications for covalent metal-oxide bonds
journal, January 2006


The α-γ transition in cerium is a Mott transition
journal, September 1974


Orbital-selective Mott-insulator transition in Ca 2 - x Sr x RuO 4
journal, February 2002