Phonon density of states for α-plutonium from density-functional theory

Söderlind, Per; Yang, Lin H.

doi:10.1038/s41598-019-55343-z

Title: Phonon density of states for α-plutonium from density-functional theory

Journal Article · 09 December 2019 · Scientific Reports

DOI: https://doi.org/10.1038/s41598-019-55343-z · OSTI ID:1607846

Söderlind, Per ^[1]; Yang, Lin H. ^[1]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

The ground-state α phase of plutonium has an extraordinary 16-atom per cell, monoclinic crystal structure defined by 20 parameters, including the cell dimensions, not dictated by the symmetry. The electronic, magnetic, and elastic properties of this complicated material have been predicted in the past but here we compute its phonon spectra. Employing a density-functional-theory (DFT) model, that is fully relativistic and accounts for orbital–orbital coupling (orbital polarization, OP), we determine the phonon density of states of α-plutonium and find good agreement with inelastic x-ray scattering. The calculated specific heat also compares very favorably with experiment. An analysis of the partial atom-projected phonon spectra suggests that atom type 8, that is located in a more open space of the structure, dominates the intensity at very high phonon frequencies. This feature of the model is essential for a good agreement with the experimental spectra. The satisfactory comparison between theory and experiment for the phonons and specific heat suggests that the DFT (+OP) approach is appropriate and accurate for α-plutonium.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1607846

Report Number(s):: LLNL-JRNL-789105; 987406

Journal Information:: Scientific Reports, Journal Name: Scientific Reports Journal Issue: 1 Vol. 9; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (49)

PHON: A program to calculate phonons using the small displacement method Alfè, Dario Computer Physics Communications, Vol. 180, Issue 12 https://doi.org/10.1016/j.cpc.2009.03.010	journal	December 2009
Thermodynamic, alloying and defect properties of plutonium: Density-functional calculations Robert, G.; Pasturel, A.; Siberchicot, B. Journal of Alloys and Compounds, Vol. 444-445 https://doi.org/10.1016/j.jallcom.2006.09.118	journal	October 2007
Temperature and time-dependence of the elastic moduli of Pu and Pu–Ga alloys Migliori, Albert; Mihut, I.; Betts, J. B. Journal of Alloys and Compounds, Vol. 444-445 https://doi.org/10.1016/j.jallcom.2006.11.157	journal	October 2007
X-ray diffraction study of pure plutonium under pressure Faure, Ph.; Genestier, C. Journal of Nuclear Materials, Vol. 385, Issue 1 https://doi.org/10.1016/j.jnucmat.2008.10.038	journal	March 2009
Correlated electrons in δ-plutonium within a dynamical mean-field picture Savrasov, S. Y.; Kotliar, G.; Abrahams, E. Nature, Vol. 410, Issue 6830 https://doi.org/10.1038/35071035	journal	April 2001
Fluctuating valence in a correlated solid and the anomalous properties of δ-plutonium Shim, J. H.; Haule, K.; Kotliar, G. Nature, Vol. 446, Issue 7135 https://doi.org/10.1038/nature05647	journal	March 2007
(Fe,Ni)2P allabogdanite can be an ambient pressure phase in iron meteorites Litasov, Konstantin D.; Bekker, Tatyana B.; Sagatov, Nursultan E. Scientific Reports, Vol. 10, Issue 1 https://doi.org/10.1038/s41598-020-66039-0	journal	June 2020
Phonon and magnetic structure in δ-plutonium from density-functional theory Söderlind, Per; Zhou, F.; Landa, A. Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep15958	journal	October 2015
Origin of the multiple configurations that drive the response of δ-plutonium’s elastic moduli to temperature Migliori, Albert; Söderlind, Per; Landa, Alexander Proceedings of the National Academy of Sciences, Vol. 113, Issue 40 https://doi.org/10.1073/pnas.1609215113	journal	September 2016
Density-functional theory for plutonium Söderlind, Per; Landa, A.; Sadigh, B. Advances in Physics, Vol. 68, Issue 1 https://doi.org/10.1080/00018732.2019.1599554	journal	January 2019
Calculated thermodynamic properties of plutonium metal Robert, G.; Pasturel, A.; Siberchicot, B. Journal of Physics: Condensed Matter, Vol. 15, Issue 49 https://doi.org/10.1088/0953-8984/15/49/015	journal	November 2003
A unified and efficient theory for the structural properties of actinides and phases of plutonium Amadon, Bernard; Dorado, Boris Journal of Physics: Condensed Matter, Vol. 30, Issue 40 https://doi.org/10.1088/1361-648x/aadc7a	journal	September 2018
Quantifying the importance of orbital over spin correlations in δ − Pu within density-functional theory Söderlind, Per Physical Review B, Vol. 77, Issue 8 https://doi.org/10.1103/physrevb.77.085101	journal	February 2008
First-principles DFT+DMFT calculations of structural properties of actinides: Role of Hund's exchange, spin-orbit coupling, and crystal structure Amadon, Bernard Physical Review B, Vol. 94, Issue 11 https://doi.org/10.1103/physrevb.94.115148	journal	September 2016
Multiplet effects in the electronic structure of δ-Pu, Am and their compounds Shick, A.; Kolorenč, J.; Havela, L. Europhysics Letters (EPL), Vol. 77, Issue 1 https://doi.org/10.1209/0295-5075/77/17003	journal	January 2007
Ambient pressure phase diagram of plutonium: A unified theory for α-Pu and δ-Pu Söderlind, P. Europhysics Letters (EPL), Vol. 55, Issue 4 https://doi.org/10.1209/epl/i2001-00447-3	journal	August 2001
Computational modeling of actinide materials and complexes Söderlind, Per; Kotliar, G.; Haule, K. MRS Bulletin, Vol. 35, Issue 11 https://doi.org/10.1557/mrs2010.715	journal	November 2010
Novel electronic configuration in ∂−Pu Eriksson, Olle; Becker, J. D.; Balatsky, A. V. Journal of Alloys and Compounds, Vol. 287, Issue 1-2 https://doi.org/10.1016/S0925-8388(99)00063-8	journal	June 1999
PHON: A program to calculate phonons using the small displacement method Alfè, Dario Computer Physics Communications, Vol. 180, Issue 12 https://doi.org/10.1016/j.cpc.2009.03.010	journal	December 2009
Thermodynamic, alloying and defect properties of plutonium: Density-functional calculations Robert, G.; Pasturel, A.; Siberchicot, B. Journal of Alloys and Compounds, Vol. 444-445 https://doi.org/10.1016/j.jallcom.2006.09.118	journal	October 2007
Temperature and time-dependence of the elastic moduli of Pu and Pu–Ga alloys Migliori, Albert; Mihut, I.; Betts, J. B. Journal of Alloys and Compounds, Vol. 444-445 https://doi.org/10.1016/j.jallcom.2006.11.157	journal	October 2007
X-ray diffraction study of pure plutonium under pressure Faure, Ph.; Genestier, C. Journal of Nuclear Materials, Vol. 385, Issue 1 https://doi.org/10.1016/j.jnucmat.2008.10.038	journal	March 2009
First principles phonon calculations in materials science Togo, Atsushi; Tanaka, Isao Scripta Materialia, Vol. 108 https://doi.org/10.1016/j.scriptamat.2015.07.021	journal	November 2015
Correlated electrons in δ-plutonium within a dynamical mean-field picture Savrasov, S. Y.; Kotliar, G.; Abrahams, E. Nature, Vol. 410, Issue 6830 https://doi.org/10.1038/35071035	journal	April 2001
Fluctuating valence in a correlated solid and the anomalous properties of δ-plutonium Shim, J. H.; Haule, K.; Kotliar, G. Nature, Vol. 446, Issue 7135 https://doi.org/10.1038/nature05647	journal	March 2007
Lattice dynamics and elasticity for ε-plutonium Söderlind, Per Scientific Reports, Vol. 7, Issue 1 https://doi.org/10.1038/s41598-017-01034-6	journal	April 2017
Physical mechanism of δ-δ′-ε phase stability in plutonium Li, Chun-Mei; Johansson, Börje; Vitos, Levente Scientific Reports, Vol. 7, Issue 1 https://doi.org/10.1038/s41598-017-06009-1	journal	July 2017
Phonon and magnetic structure in δ-plutonium from density-functional theory Söderlind, Per; Zhou, F.; Landa, A. Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep15958	journal	October 2015
Origin of the multiple configurations that drive the response of δ-plutonium’s elastic moduli to temperature Migliori, Albert; Söderlind, Per; Landa, Alexander Proceedings of the National Academy of Sciences, Vol. 113, Issue 40 https://doi.org/10.1073/pnas.1609215113	journal	September 2016
Density-functional theory for plutonium Söderlind, Per; Landa, A.; Sadigh, B. Advances in Physics, Vol. 68, Issue 1 https://doi.org/10.1080/00018732.2019.1599554	journal	January 2019
Theoretical aspects of the magnetism in the ferromagnetic A Fe 2 systems ( A =U, Np, Pu, and Am) Eriksson, Olle; Brooks, M. S. S.; Johansson, Börje Physical Review B, Vol. 41, Issue 13 https://doi.org/10.1103/PhysRevB.41.9087	journal	May 1990
Relativistic effects on the thermal expansion of the actinide elements Söderlind, Per; Nordström, Lars Physical Review B, Vol. 42, Issue 7 https://doi.org/10.1103/PhysRevB.42.4544	journal	September 1990
Structural properties of plutonium from first-principles theory Söderlind, Per; Wills, J. M.; Johansson, B. Physical Review B, Vol. 55, Issue 4 https://doi.org/10.1103/PhysRevB.55.1997	journal	January 1997
Electronic and phonon properties of six crystalline phases of Pu metal Wallace, Duane C. Physical Review B, Vol. 58, Issue 23 https://doi.org/10.1103/PhysRevB.58.15433	journal	December 1998
Dynamical mean-field theory investigation of specific heat and electronic structure of α - and δ -plutonium Pourovskii, L. V.; Kotliar, G.; Katsnelson, M. I. Physical Review B, Vol. 75, Issue 23 https://doi.org/10.1103/PhysRevB.75.235107	journal	June 2007
Quantifying the importance of orbital over spin correlations in δ − Pu within density-functional theory Söderlind, Per Physical Review B, Vol. 77, Issue 8 https://doi.org/10.1103/PhysRevB.77.085101	journal	February 2008
Phonon density of states of α - and δ -plutonium by inelastic x-ray scattering Manley, M. E.; Said, A. H.; Fluss, M. J. Physical Review B, Vol. 79, Issue 5 https://doi.org/10.1103/PhysRevB.79.052301	journal	February 2009
Elastic properties of Pu metal and Pu-Ga alloys Söderlind, Per; Landa, Alex; Klepeis, J. E. Physical Review B, Vol. 81, Issue 22 https://doi.org/10.1103/PhysRevB.81.224110	journal	June 2010
High-temperature phonon stabilization of γ -uranium from relativistic first-principles theory Söderlind, Per; Grabowski, B.; Yang, L. Physical Review B, Vol. 85, Issue 6 https://doi.org/10.1103/PhysRevB.85.060301	journal	February 2012
Unified character of correlation effects in unconventional Pu-based superconductors and δ -Pu Shick, A. B.; Kolorenc, J.; Rusz, J. Physical Review B, Vol. 87, Issue 2 https://doi.org/10.1103/PhysRevB.87.020505	journal	January 2013
First-principles DFT+DMFT calculations of structural properties of actinides: Role of Hund's exchange, spin-orbit coupling, and crystal structure Amadon, Bernard Physical Review B, Vol. 94, Issue 11 https://doi.org/10.1103/PhysRevB.94.115148	journal	September 2016
Ground State Theory of δ − Pu Savrasov, S. Y.; Kotliar, G. Physical Review Letters, Vol. 84, Issue 16 https://doi.org/10.1103/PhysRevLett.84.3670	journal	April 2000
Experimental Electronic Heat Capacities of α - and δ -Plutonium: Heavy-Fermion Physics in an Element Lashley, J. C.; Singleton, J.; Migliori, A. Physical Review Letters, Vol. 91, Issue 20 https://doi.org/10.1103/PhysRevLett.91.205901	journal	November 2003
Density-Functional Calculations of α , β , γ , δ , δ ′ , and ϵ Plutonium Söderlind, Per; Sadigh, Babak Physical Review Letters, Vol. 92, Issue 18 https://doi.org/10.1103/PhysRevLett.92.185702	journal	May 2004
The crystal structure of alpha plutonium metal Zachariasen, W. H.; Ellinger, F. H. Acta Crystallographica, Vol. 16, Issue 8 https://doi.org/10.1107/S0365110X63002012	journal	August 1963
Calculated Phonon Spectra of Plutonium at High Temperatures Dai, X. Science, Vol. 300, Issue 5621 https://doi.org/10.1126/science.1083428	journal	May 2003
Multiplet effects in the electronic structure of δ-Pu, Am and their compounds Shick, A.; Kolorenč, J.; Havela, L. Europhysics Letters (EPL), Vol. 77, Issue 1 https://doi.org/10.1209/0295-5075/77/17003	journal	January 2007
Ambient pressure phase diagram of plutonium: A unified theory for α-Pu and δ-Pu Söderlind, P. Europhysics Letters (EPL), Vol. 55, Issue 4 https://doi.org/10.1209/epl/i2001-00447-3	journal	August 2001
Computational modeling of actinide materials and complexes Söderlind, Per; Kotliar, G.; Haule, K. MRS Bulletin, Vol. 35, Issue 11 https://doi.org/10.1557/mrs2010.715	journal	November 2010

Similar Records

Lattice dynamics and thermodynamics for δ -plutonium from density functional theory

Journal Article · 2023 · Physical Review. B · OSTI ID:2007274

Söderlind, Per; Landa, A.; Yang, L. H.; +2 more

Phonon and magnetic structure in δ-plutonium from density-functional theory

Journal Article · 2015 · Scientific Reports · OSTI ID:1262182

Söderlind, Per; Zhou, F.; Landa, A.; +1 more

Mechanical and Thermal Properties for Uranium and U–6Nb Alloy from First-Principles Theory

Journal Article · 2021 · Applied Sciences · OSTI ID:1815361

Söderlind, Per; Yang, Lin H.; Landa, Alexander; +1 more

Related Subjects

75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
Physics - Condensed matter physics

Title: Phonon density of states for α-plutonium from density-functional theory

Citation Formats

References (49)

Similar Records

Related Subjects