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}
}
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