The valence-fluctuating ground state of plutonium
Abstract
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.
- Authors:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Rutgers Univ., Piscataway, NJ (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Institute for Transuranium Elements, Karlsruhe (Germany)
- Publication Date:
- Research Org.:
- 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 Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1236683
- Report Number(s):
- LA-UR-15-20256
Journal ID: ISSN 2375-2548
- Grant/Contract Number:
- AC52-06NA25396
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Science Advances
- Additional Journal Information:
- Journal Volume: 1; Journal Issue: 6; Journal ID: ISSN 2375-2548
- Publisher:
- AAAS
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; plutonium; valence fluctuations; electronic ground state; strongly correlated electron physics; material science; Kondo physics; dynamical mean field theory; neutron spectroscopy
Citation Formats
Janoschek, Marc, Das, Pinaki, Chakrabarti, Bismayan, Abernathy, Douglas L., Lumsden, Mark D., Lawrence, John M., Thompson, Joe D., Lander, Gerard H., Mitchell, Jeremy N., Richmond, Scott, Ramos, Mike, Trouw, Frans, Zhu, Jian -Xin, Haule, Kristjan, Kotliar, Gabriel, and Bauer, Eric D. The valence-fluctuating ground state of plutonium. United States: N. p., 2015.
Web. doi:10.1126/sciadv.1500188.
Janoschek, Marc, Das, Pinaki, Chakrabarti, Bismayan, Abernathy, Douglas L., Lumsden, Mark D., Lawrence, John M., Thompson, Joe D., Lander, Gerard H., Mitchell, Jeremy N., Richmond, Scott, Ramos, Mike, Trouw, Frans, Zhu, Jian -Xin, Haule, Kristjan, Kotliar, Gabriel, & Bauer, Eric D. The valence-fluctuating ground state of plutonium. United States. https://doi.org/10.1126/sciadv.1500188
Janoschek, Marc, Das, Pinaki, Chakrabarti, Bismayan, Abernathy, Douglas L., Lumsden, Mark D., Lawrence, John M., Thompson, Joe D., Lander, Gerard H., Mitchell, Jeremy N., Richmond, Scott, Ramos, Mike, Trouw, Frans, Zhu, Jian -Xin, Haule, Kristjan, Kotliar, Gabriel, and Bauer, Eric D. Fri .
"The valence-fluctuating ground state of plutonium". United States. https://doi.org/10.1126/sciadv.1500188. https://www.osti.gov/servlets/purl/1236683.
@article{osti_1236683,
title = {The valence-fluctuating ground state of plutonium},
author = {Janoschek, Marc and Das, Pinaki and Chakrabarti, Bismayan and Abernathy, Douglas L. and Lumsden, Mark D. and Lawrence, John M. and Thompson, Joe D. and Lander, Gerard H. and Mitchell, Jeremy N. and Richmond, Scott and Ramos, Mike and Trouw, Frans and Zhu, Jian -Xin and Haule, Kristjan and Kotliar, Gabriel and Bauer, Eric D.},
abstractNote = {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.},
doi = {10.1126/sciadv.1500188},
journal = {Science Advances},
number = 6,
volume = 1,
place = {United States},
year = {Fri Jul 10 00:00:00 EDT 2015},
month = {Fri Jul 10 00:00:00 EDT 2015}
}
Web of Science
Works referenced in this record:
Limits for ordered magnetism in Pu from muon spin rotation spectroscopy
journal, March 2006
- Heffner, R. H.; Morris, G. D.; Fluss, M. J.
- Physical Review B, Vol. 73, Issue 9
Inelastic neutron scattering in single-crystal
journal, June 1997
- Lawrence, J. M.; Shapiro, S. M.; Sarrao, J. L.
- Physical Review B, Vol. 55, Issue 21
Neutron Magnetic Form Factor in Strongly Correlated Materials
journal, January 2011
- Pezzoli, Maria Elisabetta; Haule, Kristjan; Kotliar, Gabriel
- Physical Review Letters, Vol. 106, Issue 1
Recent advances in magnetic structure determination by neutron powder diffraction
journal, October 1993
- Rodríguez-Carvajal, Juan
- Physica B: Condensed Matter, Vol. 192, Issue 1-2
- transition in cerium: Magnetic form factor and dynamic magnetic susceptibility in dynamical mean-field theory
journal, March 2014
- Chakrabarti, B.; Pezzoli, M. E.; Sordi, G.
- Physical Review B, Vol. 89, Issue 12
Atomistic modeling of thermodynamic properties of Pu-Ga alloys based on the Invar mechanism
journal, May 2014
- Lee, Tongsik; Taylor, Christopher D.; Lawson, A. C.
- Physical Review B, Vol. 89, Issue 17
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
Electronic structure calculations with dynamical mean-field theory
journal, August 2006
- Kotliar, G.; Savrasov, S. Y.; Haule, K.
- Reviews of Modern Physics, Vol. 78, Issue 3
Neutron self-shielding factors for simple geometrics
journal, November 1982
- Fleming, Ronald F.
- The International Journal of Applied Radiation and Isotopes, Vol. 33, Issue 11
Dynamical mean-field theory within the full-potential methods: Electronic structure of , , and
journal, May 2010
- Haule, Kristjan; Yee, Chuck-Hou; Kim, Kyoo
- Physical Review B, Vol. 81, Issue 19
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
Q -dependence of the spin fluctuations in the intermediate valence compound CePd 3
journal, May 2014
- Fanelli, V. R.; Lawrence, J. M.; Goremychkin, E. A.
- Journal of Physics: Condensed Matter, Vol. 26, Issue 22
Absence of magnetic moments in plutonium
journal, August 2005
- Lashley, J. C.; Lawson, A.; McQueeney, R. J.
- Physical Review B, Vol. 72, Issue 5
Magnetism or bonding: A nearly periodic table of transition elements
journal, March 1983
- Smith, J. L.; Kmetko, E. A.
- Journal of the Less Common Metals, Vol. 90, Issue 1
Fluctuating valence in a correlated solid and the anomalous properties of δ-plutonium
journal, March 2007
- Shim, J. H.; Haule, K.; Kotliar, G.
- Nature, Vol. 446, Issue 7135
Quantum Monte Carlo impurity solver for cluster dynamical mean-field theory and electronic structure calculations with adjustable cluster base
journal, April 2007
- Haule, Kristjan
- Physical Review B, Vol. 75, Issue 15
$α-γ$ transition in cerium: magnetic form factor and dynamic magnetic susceptibility in dynamical mean-field theory
text, January 2014
- Chakrabarti, B.; Pezzoli, M. E.; Sordi, G.
- arXiv
Magnetic correlations and neutron scattering
journal, July 1968
- Marshall, W.; Lowde, R. D.
- Reports on Progress in Physics, Vol. 31, Issue 2
Localized Magnetic States in Metals
journal, October 1961
- Anderson, P. W.
- Physical Review, Vol. 124, Issue 1
Intermultiplet transitions using neutron spectroscopy
book, January 1991
- Osborn, R.; Lovesey, S. W.; Taylor, A. D.
- Handbook on the Physics and Chemistry of Rare Earths
Experimental electronic heat capacities of $α-$ and $δ-$Plutonium; heavy-fermion physics in an element
text, January 2003
- Lashley, J. C.; Singleton, J.; Migliori, A.
- arXiv
Nature of the states in actinide metals
journal, February 2009
- Moore, Kevin T.; van der Laan, Gerrit
- Reviews of Modern Physics, Vol. 81, Issue 1
Experimental Electronic Heat Capacities of - and -Plutonium: Heavy-Fermion Physics in an Element
journal, November 2003
- Lashley, J. C.; Singleton, J.; Migliori, A.
- Physical Review Letters, Vol. 91, Issue 20
Absolute cross-section normalization of magnetic neutron scattering data
journal, August 2013
- Xu, Guangyong; Xu, Zhijun; Tranquada, J. M.
- Review of Scientific Instruments, Vol. 84, Issue 8
Emergent states in heavy-electron materials
journal, September 2012
- Yang, Y. -f.; Pines, D.
- Proceedings of the National Academy of Sciences, Vol. 109, Issue 45
Unusual Phonon Softening in -Phase Plutonium
journal, April 2004
- McQueeney, R. J.; Lawson, A. C.; Migliori, A.
- Physical Review Letters, Vol. 92, Issue 14
Analytic results on dynamics of the degenerate Anderson model
journal, October 1985
- Kuramoto, Y.; Müller-Hartmann, E.
- Journal of Magnetism and Magnetic Materials, Vol. 52, Issue 1-4
Multiconfigurational nature of 5f orbitals in uranium and plutonium intermetallics
text, January 2012
- Booth, C. H.; Jiang, Yu; Wang, D. L.
- arXiv
Valence fluctuations in thin films and the and phases of Pu metal determined by core-level photoemission calculations
journal, July 2010
- van der Laan, G.; Taguchi, M.
- Physical Review B, Vol. 82, Issue 4
Design and operation of the wide angular-range chopper spectrometer ARCS at the Spallation Neutron Source
journal, January 2012
- Abernathy, D. L.; Stone, M. B.; Loguillo, M. J.
- Review of Scientific Instruments, Vol. 83, Issue 1
Electronic Energy Levels of the Lighter Actinides: U 3+ , Np 3+ , Pu 3+ , Am 3+ , and Cm 3+
journal, June 1964
- Carnall, W. T.; Wybourne, B. G.
- The Journal of Chemical Physics, Vol. 40, Issue 11
The strong-correlations puzzle
journal, June 2009
- Quintanilla, Jorge; Hooley, Chris
- Physics World, Vol. 22, Issue 06
Neutron magnetic form factor in strongly correlated materials
text, January 2010
- Pezzoli, Maria Elisabetta; Haule, Kristjan; Kotliar, Gabriel
- arXiv
Relation between the Anderson and Kondo Hamiltonians
journal, September 1966
- Schrieffer, J. R.; Wolff, P. A.
- Physical Review, Vol. 149, Issue 2
The solubility of hydrogen and deuterium in alloyed, unalloyed and impure plutonium metal
journal, March 2010
- Richmond, S.; Bridgewater, J. S.; Ward, J. W.
- IOP Conference Series: Materials Science and Engineering, Vol. 9
The magnetic susceptibility of Americium and curium metal
journal, September 1975
- Kanellakopulos, B.; Blaise, A.; Fournier, J. M.
- Solid State Communications, Vol. 17, Issue 6
Spin dynamics in the mixed valence alloy
journal, September 1977
- Shapiro, S. M.; Axe, J. D.; Birgeneau, R. J.
- Physical Review B, Vol. 16, Issue 5
Pu neutron scattering studies – Magnetism and structure
journal, March 2009
- Trouw, F.; Rhyne, J. J.; Mitchell, J. N.
- Journal of Nuclear Materials, Vol. 385, Issue 1
The plutonium-gallium system
journal, July 1964
- Ellinger, F. H.; Land, C. C.; Struebing, V. O.
- Journal of Nuclear Materials, Vol. 12, Issue 2
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
Analytic results on dynamics of the degenerate Anderson model
journal, October 1985
- Kuramoto, Y.; Müller-Hartmann, E.
- Journal of Magnetism and Magnetic Materials, Vol. 52, Issue 1-4
Design and operation of the wide angular-range chopper spectrometer ARCS at the Spallation Neutron Source
journal, January 2012
- Abernathy, D. L.; Stone, M. B.; Loguillo, M. J.
- Review of Scientific Instruments, Vol. 83, Issue 1
Absolute cross-section normalization of magnetic neutron scattering data
journal, August 2013
- Xu, Guangyong; Xu, Zhijun; Tranquada, J. M.
- Review of Scientific Instruments, Vol. 84, Issue 8
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
Emergent states in heavy-electron materials
journal, September 2012
- Yang, Y. -f.; Pines, D.
- Proceedings of the National Academy of Sciences, Vol. 109, Issue 45
Q -dependence of the spin fluctuations in the intermediate valence compound CePd 3
journal, May 2014
- Fanelli, V. R.; Lawrence, J. M.; Goremychkin, E. A.
- Journal of Physics: Condensed Matter, Vol. 26, Issue 22
Magnetic Form Factor of -Ce: Towards Understanding the Magnetism of Cerium
journal, December 2005
- Murani, A. P.; Levett, S. J.; Taylor, J. W.
- Physical Review Letters, Vol. 95, Issue 25
Works referencing / citing this record:
Pressure-driven localized-itinerant transition and valence fluctuation in cubic phase californium
journal, January 2019
- Huang, Li; Lu, Haiyan
- Physical Review B, Vol. 99, Issue 4
Phonon and magnetic structure in δ-plutonium from density-functional theory
journal, October 2015
- Söderlind, Per; Zhou, F.; Landa, A.
- Scientific Reports, Vol. 5, Issue 1
Valence fluctuation for f electrons in XGaO3 (X = Pu, Ce): a perspective from dynamic mean field theory
journal, October 2019
- Li, Ru-song; Lu, Xing; Xin, Du-qiang
- Journal of Radioanalytical and Nuclear Chemistry, Vol. 322, Issue 3
Lattice dynamics and elasticity for ε-plutonium
journal, April 2017
- Söderlind, Per
- Scientific Reports, Vol. 7, Issue 1
Electronic correlations in cerium’s high-pressure phases
journal, September 2018
- Lu, Haiyan; Huang, Li
- Journal of Physics: Condensed Matter, Vol. 30, Issue 39
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
Characterization of berkelium(III) dipicolinate and borate compounds in solution and the solid state
journal, August 2016
- Silver, M. A.; Cary, S. K.; Johnson, J. A.
- Science, Vol. 353, Issue 6302
A unified and efficient theory for the structural properties of actinides and phases of plutonium
journal, September 2018
- Amadon, Bernard; Dorado, Boris
- Journal of Physics: Condensed Matter, Vol. 30, Issue 40
Thermodynamics of the bulk modulus of delta phase plutonium alloys
journal, March 2019
- Lawson, A. C.
- Philosophical Magazine, Vol. 99, Issue 12
Instability of the f -electron state in URu 2 Si 2 − x P x probed using high magnetic fields
journal, June 2019
- Huang, K.; Chen, K. -W.; Gallagher, A.
- Physical Review B, Vol. 99, Issue 23
Magnetic order and valence fluctuation in a PuGa intermetallic compound studied via a first principles calculation
journal, November 2019
- Li, Ru‐song; Lu, Xing; Xin, Du‐qiang
- International Journal of Quantum Chemistry, Vol. 120, Issue 4
Oxidation states and ionicity
journal, October 2018
- Walsh, Aron; Sokol, Alexey A.; Buckeridge, John
- Nature Materials, Vol. 17, Issue 11
Toward a predictive theory of correlated materials
journal, July 2018
- Kent, Paul R. C.; Kotliar, Gabriel
- Science, Vol. 361, Issue 6400
Phase stabilization by electronic entropy in plutonium
journal, July 2019
- Harrison, N.; Betts, J. B.; Wartenbe, M. R.
- Nature Communications, Vol. 10, Issue 1
Density-functional theory for plutonium
journal, January 2019
- Söderlind, Per; Landa, A.; Sadigh, B.
- Advances in Physics, Vol. 68, Issue 1
Site and orbital selective correlations in $β$-Pu
text, January 2018
- Brito, W. H.; Kotliar, G.
- arXiv
Isochronal annealing effects on local structure, crystalline fraction, and undamaged region size of radiation damage in Ga-stabilized δ -Pu
journal, July 2016
- Olive, D. T.; Wang, D. L.; Booth, C. H.
- Journal of Applied Physics, Vol. 120, Issue 3
Observation of 5f intermediate coupling in uranium x-ray emission spectroscopy
journal, January 2020
- Tobin, J. G.; Nowak, S.; Yu, S-W
- Journal of Physics Communications, Vol. 4, Issue 1
Anomalous thermodynamic properties and phase stability of alloys from first-principles calculations
journal, December 2016
- Li, Chun-Mei; Yang, Rui; Johansson, Börje
- Physical Review B, Vol. 94, Issue 21
Electronic and vibrational properties of : A first-principles study
journal, November 2019
- Li, Menglei; Yang, Yu; Zheng, Fawei
- Physical Review B, Vol. 100, Issue 18
Phase stabilization by electronic entropy in plutonium
journal, July 2019
- Harrison, N.; Betts, J. B.; Wartenbe, M. R.
- Nature Communications, Vol. 10, Issue 1
Lattice dynamics and elasticity for ε-plutonium
journal, April 2017
- Söderlind, Per
- Scientific Reports, Vol. 7, Issue 1
Phonon and magnetic structure in δ-plutonium from density-functional theory
journal, October 2015
- Söderlind, Per; Zhou, F.; Landa, A.
- Scientific Reports, Vol. 5, Issue 1