The valence-fluctuating ground state of plutonium

Marc Janoschek; Pinaki Das; Bismayan Chakrabarti; Douglas L. Abernathy; Mark D. Lumsden; John M. Lawrence; Joe D. Thompson; Gerard H. Lander; Jeremy N. Mitchell; Scott Richmond; Mike Ramos; Frans Trouw; Jian Xin Zhu; Kristjan Haule; Gabriel Kotliar; Eric D. Bauer

doi:10.1126/sciadv.1500188

The valence-fluctuating ground state of plutonium

Marc Janoschek, Pinaki Das, Bismayan Chakrabarti, Douglas L. Abernathy, Mark D. Lumsden, John M. Lawrence, Joe D. Thompson, Gerard H. Lander, Jeremy N. Mitchell, Scott Richmond, Mike Ramos, Frans Trouw, Jian Xin Zhu, Kristjan Haule, Gabriel Kotliar, Eric D. Bauer

Research output: Contribution to journal › Article › peer-review

102 Scopus citations

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. 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 magnetismbut also suggest an improved understanding of the effects of such electronic dichotomy in complex materials.

Original language	English
Article number	e1500188
Journal	Science Advances
Volume	1
Issue number	6
DOIs	https://doi.org/10.1126/sciadv.1500188
State	Published - Jul 2015

Funding

Work at LANL was performed under the auspices of the U.S. Department of Energy (DOE). MJ., P.D., and E.D.B. were funded by the LANL Directed Research and Development program. J.D.T. was funded by the DOE, Office of Basic Energy Sciences (BES). LANL is operated by Los Alamos National Security for the National Nuclear Security Administration of DOE under contract DE-AC52-06NA25396. Research conducted at ORNL Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences (BES), U.S. DOE. This research used resources of the Oak Ridge Leadership Computing Facility at ORNL, which is supported by the Office of Science of the U.S. DOE under Contract No. DE-AC05-00OR22725. K.H. and B.C. are supported by National Science Foundation grant DMR-1405303. G.K. is supported by BES-DOE grant DE-FG02-99ER45761. G.H.L. acknowledges support by the Seaborg Institute at LANL.

Funders	Funder number
U.S. Department of Energy
Directorate for Mathematical and Physical Sciences	1405303
British Ecological Society
National Science Foundation	DMR-1405303

Access to Document

10.1126/sciadv.1500188

Cite this

@article{f2806d91347042869cf19c92c8e5bf83,

title = "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. 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 magnetismbut also suggest an improved understanding of the effects of such electronic dichotomy in complex materials.",

author = "Marc Janoschek and Pinaki Das and Bismayan Chakrabarti 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 Scott Richmond and Mike Ramos and Frans Trouw and Zhu, {Jian Xin} and Kristjan Haule and Gabriel Kotliar and Bauer, {Eric D.}",

note = "Publisher Copyright: {\textcopyright} 2015 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).",

year = "2015",

month = jul,

doi = "10.1126/sciadv.1500188",

language = "English",

volume = "1",

journal = "Science Advances",

issn = "2375-2548",

publisher = "American Association for the Advancement of Science",

number = "6",

}

TY - JOUR

T1 - The valence-fluctuating ground state of plutonium

AU - Janoschek, Marc

AU - Das, Pinaki

AU - Chakrabarti, Bismayan

AU - Abernathy, Douglas L.

AU - Lumsden, Mark D.

AU - Lawrence, John M.

AU - Thompson, Joe D.

AU - Lander, Gerard H.

AU - Mitchell, Jeremy N.

AU - Richmond, Scott

AU - Ramos, Mike

AU - Trouw, Frans

AU - Zhu, Jian Xin

AU - Haule, Kristjan

AU - Kotliar, Gabriel

AU - Bauer, Eric D.

N1 - Publisher Copyright: © 2015 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

PY - 2015/7

Y1 - 2015/7

N2 - 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. 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 magnetismbut also suggest an improved understanding of the effects of such electronic dichotomy in complex materials.

AB - 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. 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 magnetismbut also suggest an improved understanding of the effects of such electronic dichotomy in complex materials.

UR - http://www.scopus.com/inward/record.url?scp=84973621677&partnerID=8YFLogxK

U2 - 10.1126/sciadv.1500188

DO - 10.1126/sciadv.1500188

M3 - Article

AN - SCOPUS:84973621677

SN - 2375-2548

VL - 1

JO - Science Advances

JF - Science Advances

IS - 6

M1 - e1500188

ER -

The valence-fluctuating ground state of plutonium

Abstract

Funding

Access to Document

Other files and links

Fingerprint

Cite this