Phonon and magnetic structure in δ-plutonium from density-functional theory
Abstract
We present phonon properties of plutonium metal obtained from a combination of density-functional-theory (DFT) electronic structure and the recently developed compressive sensing lattice dynamics (CSLD). The CSLD model is here trained on DFT total energies of several hundreds of quasi-random atomic configurations for best possible accuracy of the phonon properties. The calculated phonon dispersions compare better with experiment than earlier results obtained from dynamical mean-field theory. The density-functional model of the electronic structure consists of disordered magnetic moments with all relativistic effects and explicit orbital-orbital correlations. The magnetic disorder is approximated in two ways: (i) a special quasi-random structure and (ii) the disordered-local-moment (DLM) method within the coherent potential approximation. Magnetism in plutonium has been debated intensely, However, the present magnetic approach for plutonium is validated by the close agreement between the predicted magnetic form factor and that of recent neutron-scattering experiments.
- Authors:
-
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1262182
- Report Number(s):
- LLNL-JRNL-676061
Journal ID: ISSN 2045-2322
- Grant/Contract Number:
- AC52-07NA27344
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Scientific Reports
- Additional Journal Information:
- Journal Volume: 5; Journal ID: ISSN 2045-2322
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Electronic properties and materials; Magnetic materials
Citation Formats
Söderlind, Per, Zhou, F., Landa, A., and Klepeis, J. E. Phonon and magnetic structure in δ-plutonium from density-functional theory. United States: N. p., 2015.
Web. doi:10.1038/srep15958.
Söderlind, Per, Zhou, F., Landa, A., & Klepeis, J. E. Phonon and magnetic structure in δ-plutonium from density-functional theory. United States. https://doi.org/10.1038/srep15958
Söderlind, Per, Zhou, F., Landa, A., and Klepeis, J. E. Fri .
"Phonon and magnetic structure in δ-plutonium from density-functional theory". United States. https://doi.org/10.1038/srep15958. https://www.osti.gov/servlets/purl/1262182.
@article{osti_1262182,
title = {Phonon and magnetic structure in δ-plutonium from density-functional theory},
author = {Söderlind, Per and Zhou, F. and Landa, A. and Klepeis, J. E.},
abstractNote = {We present phonon properties of plutonium metal obtained from a combination of density-functional-theory (DFT) electronic structure and the recently developed compressive sensing lattice dynamics (CSLD). The CSLD model is here trained on DFT total energies of several hundreds of quasi-random atomic configurations for best possible accuracy of the phonon properties. The calculated phonon dispersions compare better with experiment than earlier results obtained from dynamical mean-field theory. The density-functional model of the electronic structure consists of disordered magnetic moments with all relativistic effects and explicit orbital-orbital correlations. The magnetic disorder is approximated in two ways: (i) a special quasi-random structure and (ii) the disordered-local-moment (DLM) method within the coherent potential approximation. Magnetism in plutonium has been debated intensely, However, the present magnetic approach for plutonium is validated by the close agreement between the predicted magnetic form factor and that of recent neutron-scattering experiments.},
doi = {10.1038/srep15958},
journal = {Scientific Reports},
number = ,
volume = 5,
place = {United States},
year = {Fri Oct 30 00:00:00 EDT 2015},
month = {Fri Oct 30 00:00:00 EDT 2015}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 46 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Atomic forces at finite magnetic temperatures: Phonons in paramagnetic iron
journal, March 2012
- Körmann, F.; Dick, A.; Grabowski, B.
- Physical Review B, Vol. 85, Issue 12
Spin-polarized relativistic linear-muffin-tin-orbital method: Volume-dependent electronic structure and magnetic moment of plutonium
journal, June 1991
- Solovyev, I. V.; Liechtenstein, A. I.; Gubanov, V. A.
- Physical Review B, Vol. 43, Issue 18
Spin-polarized relativistic linear-muffin-tin-orbital method: Volume-dependent electronic structure and magnetic moment of plutonium
journal, June 1991
- Solovyev, I. V.; Liechtenstein, A. I.; Gubanov, V. A.
- Physical Review B, Vol. 43, Issue 18
-electron Delocalization in Americium
journal, May 1980
- Skriver, H. L.; Andersen, O. K.; Johansson, B.
- Physical Review Letters, Vol. 44, Issue 18
Cerium; Crystal Structure and Position in The Periodic Table
journal, September 2014
- Johansson, Börje; Luo, Wei; Li, Sa
- Scientific Reports, Vol. 4, Issue 1
A first-principles theory of ferromagnetic phase transitions in metals
journal, June 1985
- Gyorffy, B. L.; Pindor, A. J.; Staunton, J.
- Journal of Physics F: Metal Physics, Vol. 15, Issue 6
An Introduction To Compressive Sampling
journal, March 2008
- Candes, E. J.; Wakin, M. B.
- IEEE Signal Processing Magazine, Vol. 25, Issue 2
Lattice anharmonicity and thermal conductivity from compressive sensing of first-principles calculations
text, January 2014
- Zhou, Fei; Nielson, Weston; Xia, Yi
- arXiv
Temperature dependence of the samarium magnetic form factor in SmCo 5
journal, March 1979
- Givord, D.; Laforest, J.; Schweizer, J.
- Journal of Applied Physics, Vol. 50, Issue B3
Stability of δ-Pu Alloys from First-Principles Theory.
journal, July 2003
- Landa, Alex; Soederlind, Per
- ChemInform, Vol. 34, Issue 28
Calculated Phonon Spectra of Plutonium at High Temperatures
journal, May 2003
- Dai, X.
- Science, Vol. 300, Issue 5621
Calculated Bulk Properties of the Actinide Metals
journal, July 1978
- Skriver, H. L.; Andersen, O. K.; Johansson, B.
- Physical Review Letters, Vol. 41, Issue 1
The valence-fluctuating ground state of plutonium
journal, July 2015
- Janoschek, Marc; Das, Pinaki; Chakrabarti, Bismayan
- Science Advances, Vol. 1, Issue 6
A first-principles theory of ferromagnetic phase transitions in metals
journal, June 1985
- Gyorffy, B. L.; Pindor, A. J.; Staunton, J.
- Journal of Physics F: Metal Physics, Vol. 15, Issue 6
Density-functional investigation of magnetism in -Pu
journal, November 2002
- Söderlind, Per; Landa, Alex; Sadigh, Babak
- Physical Review B, Vol. 66, Issue 20
Lattice Anharmonicity and Thermal Conductivity from Compressive Sensing of First-Principles Calculations
journal, October 2014
- Zhou, Fei; Nielson, Weston; Xia, Yi
- Physical Review Letters, Vol. 113, Issue 18
Electronic properties of f -electron metals using the generalized gradient approximation
journal, September 1994
- Söderlind, P.; Eriksson, O.; Johansson, B.
- Physical Review B, Vol. 50, Issue 11
Density-Functional Calculations of , , , , , and Plutonium
journal, May 2004
- Söderlind, Per; Sadigh, Babak
- Physical Review Letters, Vol. 92, Issue 18
Computational modeling of actinide materials and complexes
journal, November 2010
- Söderlind, Per; Kotliar, G.; Haule, K.
- MRS Bulletin, Vol. 35, Issue 11
Absence of magnetic moments in plutonium
journal, August 2005
- Lashley, J. C.; Lawson, A.; McQueeney, R. J.
- Physical Review B, Vol. 72, Issue 5
Compressive sensing as a paradigm for building physics models
journal, January 2013
- Nelson, Lance J.; Hart, Gus L. W.; Zhou, Fei
- Physical Review B, Vol. 87, Issue 3
Structural properties of plutonium from first-principles theory
journal, January 1997
- Söderlind, Per; Wills, J. M.; Johansson, B.
- Physical Review B, Vol. 55, Issue 4
Elastic properties of Pu metal and Pu-Ga alloys
journal, June 2010
- Söderlind, Per; Landa, Alex; Klepeis, J. E.
- Physical Review B, Vol. 81, Issue 22
Phonon Dispersions of fcc -Plutonium-Gallium by Inelastic X-ray Scattering
journal, August 2003
- Wong, J.
- Science, Vol. 301, Issue 5636
The valence-fluctuating ground state of plutonium
journal, July 2015
- Janoschek, Marc; Das, Pinaki; Chakrabarti, Bismayan
- Science Advances, Vol. 1, Issue 6
Chapter 117 Neutron elastic scattering from actinides and anomalous lanthanides
book, January 1993
- Lander, G. H.
- Lanthanides/Actinides: Physics I
Calculated Phonon Spectra of Plutonium at High Temperatures
journal, May 2003
- Dai, X.
- Science, Vol. 300, Issue 5621
The electronic and structural properties of δ-Pu and PuO from the LSDA (GGA)+U method
journal, September 2010
- Liu, T.; Cai, T.; Gao, T.
- Physica B: Condensed Matter, Vol. 405, Issue 17
Cerium; Crystal Structure and Position in The Periodic Table
journal, September 2014
- Johansson, Börje; Luo, Wei; Li, Sa
- Scientific Reports, Vol. 4, Issue 1
Novel electronic configuration in ∂−Pu
journal, June 1999
- Eriksson, Olle; Becker, J. D.; Balatsky, A. V.
- Journal of Alloys and Compounds, Vol. 287, Issue 1-2
Stability of δ-Pu alloys from first-principles theory
journal, May 2003
- Landa, Alex; Söderlind, Per
- Journal of Alloys and Compounds, Vol. 354, Issue 1-2
First-principles elastic constants and phonons of
journal, October 2004
- Söderlind, P.; Landa, A.; Sadigh, B.
- Physical Review B, Vol. 70, Issue 14
Works referencing / citing this record:
Phonon density of states for α-plutonium from density-functional theory
journal, December 2019
- Söderlind, Per; Yang, Lin H.
- Scientific Reports, Vol. 9, Issue 1
Quantitative Analysis of Cerium-Gallium Alloys Using a Hand-Held Laser Induced Breakdown Spectroscopy Device
journal, August 2019
- Rao, Ashwin P.; Cook, Matthew T.; Hall, Howard L.
- Atoms, Vol. 7, Issue 3
Lattice dynamics and elasticity for ε-plutonium
journal, April 2017
- Söderlind, Per
- Scientific Reports, Vol. 7, Issue 1
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
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
Compressive sensing lattice dynamics. I. General formalism
text, January 2018
- Zhou, Fei; Nielson, Weston; Xia, Yi
- arXiv
Physical mechanism of δ-δ′-ε phase stability in plutonium
journal, July 2017
- Li, Chun-Mei; Johansson, Börje; Vitos, Levente
- Scientific Reports, Vol. 7, Issue 1
Density-functional theory for plutonium
journal, January 2019
- Söderlind, Per; Landa, A.; Sadigh, B.
- Advances in Physics, Vol. 68, 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
Lattice dynamics and elasticity for ε-plutonium
journal, April 2017
- Söderlind, Per
- Scientific Reports, Vol. 7, Issue 1