High-Temperature Thermodynamics of Uranium from Ab Initio Modeling

Söderlind, Per; Landa, Alexander; Moore, Emily E.; Perron, Aurélien; Roehling, John; McKeown, Joseph T.

doi:10.3390/app13042123

Title: High-Temperature Thermodynamics of Uranium from Ab Initio Modeling

Abstract

We present high-temperature thermodynamic properties for uranium in its γ phase (γ-U) from first-principles, relativistic, and anharmonic theory. The results are compared to CALPHAD modeling. The ab initio electronic structure is obtained from density-functional theory (DFT) that includes spin–orbit coupling and an added self-consistent orbital-polarization (OP) mechanism for more accurate treatment of magnetism. The first-principles method is coupled to a lattice dynamics scheme that is used to model anharmonic lattice vibrations, namely, Self-Consistent Ab Initio Lattice Dynamics (SCAILD). The methodology can be summarized in the acronym DFT + OP + SCAILD. Upon thermal expansion, γ-U develops non-negligible magnetic moments that are included for the first time in thermodynamic theory. The all-electron DFT approach is shown to model γ-U better than the commonly used pseudopotential method. In addition to CALPHAD, DFT + OP + SCAILD thermodynamic properties are compared with other ab initio and semiempirical modeling and experiments. Our first-principles approach produces Gibbs free energy that is essentially identical to CALPHAD. The DFT + OP + SCAILD heat capacity is close to CALPHAD and most experimental data and is predicted to have a significant thermal dependence due to the electronic contribution.

Authors:

^[1];

^[1]; Roehling, John ^[1]; McKeown, Joseph T. ^[1]

Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Publication Date:: Tue Feb 07 00:00:00 EST 2023

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

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:: 1999713

Report Number(s):: LLNL-JRNL-843528
Journal ID: ISSN 2076-3417; 1066231; TRN: US2405475

Grant/Contract Number:: AC52-07NA27344

Resource Type:: Accepted Manuscript

Journal Name:: Applied Sciences

Additional Journal Information:: Journal Volume: 13; Journal Issue: 4; Journal ID: ISSN 2076-3417

Publisher:: MDPI

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; uranium; specific heat; anharmonic; first principles; CALPHAD; DFT

Citation Formats


                    Söderlind, Per, Landa, Alexander, Moore, Emily E., Perron, Aurélien, Roehling, John, and McKeown, Joseph T. High-Temperature Thermodynamics of Uranium from Ab Initio Modeling.  United States: N. p., 2023. 
Web.  doi:10.3390/app13042123.

Copy to clipboard


                    Söderlind, Per, Landa, Alexander, Moore, Emily E., Perron, Aurélien, Roehling, John, & McKeown, Joseph T. High-Temperature Thermodynamics of Uranium from Ab Initio Modeling.  United States.  https://doi.org/10.3390/app13042123

Copy to clipboard


                    Söderlind, Per, Landa, Alexander, Moore, Emily E., Perron, Aurélien, Roehling, John, and McKeown, Joseph T. Tue .  
"High-Temperature Thermodynamics of Uranium from Ab Initio Modeling".  United States.  https://doi.org/10.3390/app13042123.  https://www.osti.gov/servlets/purl/1999713.

Copy to clipboard


                    
@article{osti_1999713,

  title        = {High-Temperature Thermodynamics of Uranium from Ab Initio Modeling},

  author       = {Söderlind, Per and Landa, Alexander and Moore, Emily E. and Perron, Aurélien and Roehling, John and McKeown, Joseph T.},

  abstractNote = {We present high-temperature thermodynamic properties for uranium in its γ phase (γ-U) from first-principles, relativistic, and anharmonic theory. The results are compared to CALPHAD modeling. The ab initio electronic structure is obtained from density-functional theory (DFT) that includes spin–orbit coupling and an added self-consistent orbital-polarization (OP) mechanism for more accurate treatment of magnetism. The first-principles method is coupled to a lattice dynamics scheme that is used to model anharmonic lattice vibrations, namely, Self-Consistent Ab Initio Lattice Dynamics (SCAILD). The methodology can be summarized in the acronym DFT + OP + SCAILD. Upon thermal expansion, γ-U develops non-negligible magnetic moments that are included for the first time in thermodynamic theory. The all-electron DFT approach is shown to model γ-U better than the commonly used pseudopotential method. In addition to CALPHAD, DFT + OP + SCAILD thermodynamic properties are compared with other ab initio and semiempirical modeling and experiments. Our first-principles approach produces Gibbs free energy that is essentially identical to CALPHAD. The DFT + OP + SCAILD heat capacity is close to CALPHAD and most experimental data and is predicted to have a significant thermal dependence due to the electronic contribution.},

  doi          = {10.3390/app13042123},

  journal      = {Applied Sciences},

  number       = 4,

  volume       = 13,

  place        = {United States},

  year         = {Tue Feb 07 00:00:00 EST 2023},

  month        = {Tue Feb 07 00:00:00 EST 2023}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (DOE)

Publisher's Version of Record

https://doi.org/10.3390/app13042123

Other availability

Search WorldCat to find libraries that may hold this journal

Save / Share:

Export Metadata

Save to My Library

Works referenced in this record:

Metallic fuels for advanced reactors
journal, July 2009

Carmack, W. J.; Porter, D. L.; Chang, Y. I.
Journal of Nuclear Materials, Vol. 392, Issue 2
DOI: 10.1016/j.jnucmat.2009.03.007

Molecular-dynamic simulation of the thermophysical properties of liquid uranium
journal, June 2010

Belashchenko, D. K.; Smirnova, D. E.; Ostrovski, O. I.
High Temperature, Vol. 48, Issue 3
DOI: 10.1134/S0018151X10030107

A ternary EAM interatomic potential for U–Mo alloys with xenon
journal, March 2013

Smirnova, D. E.; Kuksin, A. Yu; Starikov, S. V.
Modelling and Simulation in Materials Science and Engineering, Vol. 21, Issue 3
DOI: 10.1088/0965-0393/21/3/035011

Atomistic simulation of defect formation and structure transitions in U-Mo alloys in swift heavy ion irradiation
journal, November 2017

Kolotova, L. N.; Starikov, S. V.
Journal of Nuclear Materials, Vol. 495
DOI: 10.1016/j.jnucmat.2017.07.044

High-temperature phonon stabilization of $γ$ -uranium from relativistic first-principles theory
journal, February 2012

Söderlind, Per; Grabowski, B.; Yang, L.
Physical Review B, Vol. 85, Issue 6
DOI: 10.1103/PhysRevB.85.060301

Entropy Driven Stabilization of Energetically Unstable Crystal Structures Explained from First Principles Theory
journal, March 2008

Souvatzis, P.; Eriksson, O.; Katsnelson, M. I.
Physical Review Letters, Vol. 100, Issue 9
DOI: 10.1103/PhysRevLett.100.095901

The atomistic simulation of pressure-induced phase transition in uranium mononitride
journal, November 2016

Tseplyaev, V. I.; Starikov, S. V.
Journal of Nuclear Materials, Vol. 480
DOI: 10.1016/j.jnucmat.2016.07.048

Orbital polarization in narrow-band systems: Application to volume collapses in light lanthanides
journal, April 1990

Eriksson, Olle; Brooks, M. S. S.; Johansson, Börje
Physical Review B, Vol. 41, Issue 10
DOI: 10.1103/PhysRevB.41.7311

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999

Kresse, G.; Joubert, D.
Physical Review B, Vol. 59, Issue 3, p. 1758-1775
DOI: 10.1103/PhysRevB.59.1758

First-principles elastic and structural properties of uranium metal
journal, August 2002

Söderlind, Per
Physical Review B, Vol. 66, Issue 8
DOI: 10.1103/PhysRevB.66.085113

Atomistic properties of γ uranium
journal, February 2012

Beeler, Benjamin; Deo, Chaitanya; Baskes, Michael
Journal of Physics: Condensed Matter, Vol. 24, Issue 7
DOI: 10.1088/0953-8984/24/7/075401

SGTE data for pure elements
journal, October 1991

Dinsdale, A. T.
Calphad, Vol. 15, Issue 4
DOI: 10.1016/0364-5916(91)90030-N

Atomistic Simulation of the Fission-Fragment-Induced Formation of Defects in a Uranium–Molybdenum Alloy
journal, July 2019

Kolotova, L. N.; Starikov, S. V.; Ozrin, V. D.
Journal of Experimental and Theoretical Physics, Vol. 129, Issue 1
DOI: 10.1134/S1063776119060128

First-principles study of bubble nucleation and growth behaviors in α U–Zr
journal, September 2012

Huang, Gui-Yang; Wirth, B. D.
Journal of Physics: Condensed Matter, Vol. 24, Issue 41
DOI: 10.1088/0953-8984/24/41/415404

Thermodynamic properties of α-uranium
journal, November 2016

Ren, Zhiyong; Wu, Jun; Ma, Rong
Journal of Nuclear Materials, Vol. 480
DOI: 10.1016/j.jnucmat.2016.08.012

The Heat Capacities of Uranium, Uranium Trioxide, and Uranium Dioxide from 15°K to 300°K
journal, April 1952

Jones, W. M.; Gordon, Joseph; Long, E. A.
The Journal of Chemical Physics, Vol. 20, Issue 4
DOI: 10.1063/1.1700518

Spin disorder in paramagnetic fcc iron
journal, June 1989

Grimvall, Göran
Physical Review B, Vol. 39, Issue 16
DOI: 10.1103/PhysRevB.39.12300

First-principles phase stability, bonding, and electronic structure of actinide metals
journal, June 2014

Söderlind, Per
Journal of Electron Spectroscopy and Related Phenomena, Vol. 194
DOI: 10.1016/j.elspec.2013.11.009

Understanding the Complex Phase Diagram of Uranium: The Role of Electron-Phonon Coupling
journal, September 2011

Raymond, S.; Bouchet, J.; Lander, G. H.
Physical Review Letters, Vol. 107, Issue 13
DOI: 10.1103/PhysRevLett.107.136401

Lattice dynamics simulation using machine learning interatomic potentials
journal, February 2020

Ladygin, V. V.; Korotaev, P. Yu.; Yanilkin, A. V.
Computational Materials Science, Vol. 172
DOI: 10.1016/j.commatsci.2019.109333

Elastic constants of cubic f -electron elements: Theory
journal, October 1993

Söderlind, Per; Eriksson, Olle; Wills, J. M.
Physical Review B, Vol. 48, Issue 13
DOI: 10.1103/PhysRevB.48.9306

Thermo-Calc & DICTRA, computational tools for materials science
journal, June 2002

Andersson, J-O; Helander, Thomas; Höglund, Lars
Calphad, Vol. 26, Issue 2
DOI: 10.1016/S0364-5916(02)00037-8

Theory of the crystal structures of cerium and the light actinides
journal, November 1998

Soderlind, Per
Advances in Physics, Vol. 47, Issue 6
DOI: 10.1080/000187398243492

Spin fluctuations in paramagnetic chromium determined from entropy considerations
journal, June 1993

Grimvall, G.; Häglund, J.; Fernández Guillermet, A.
Physical Review B, Vol. 47, Issue 22
DOI: 10.1103/PhysRevB.47.15338

Thermal evolution of vibrational properties of $α$ -U
journal, November 2015

Bouchet, J.; Bottin, F.
Physical Review B, Vol. 92, Issue 17
DOI: 10.1103/PhysRevB.92.174108

Heat capacity of metallic uranium and thorium from 80 to 1000 k
journal, January 1980

Nakamura, Jin-ichi; Takahashi, Yoichi; Izumi, Shin-ichiro
Journal of Nuclear Materials, Vol. 88, Issue 1
DOI: 10.1016/0022-3115(80)90386-4

Ab initio molecular dynamics investigation of point defects in $γ$ -U
journal, March 2021

Beeler, Benjamin; Andersson, David; Jiang, Chao
Journal of Nuclear Materials, Vol. 545
DOI: 10.1016/j.jnucmat.2020.152714

Orbital polarization in the Kohn-Sham-Dirac theory
journal, November 2005

Eschrig, H.; Sargolzaei, M.; Koepernik, K.
Europhysics Letters (EPL), Vol. 72, Issue 4
DOI: 10.1209/epl/i2005-10285-9

Many-body interatomic U and Al–U potentials
journal, May 2012

Pascuet, M. I.; Bonny, G.; Fernández, J. R.
Journal of Nuclear Materials, Vol. 424, Issue 1-3
DOI: 10.1016/j.jnucmat.2012.03.002

Atomistic modeling of the self-diffusion in γ-U and γ-U-Mo
journal, May 2015

Smirnova, D. E.; Kuksin, A. Yu.; Starikov, S. V.
The Physics of Metals and Metallography, Vol. 116, Issue 5
DOI: 10.1134/S0031918X1503014X

Density-functional theory for plutonium
journal, January 2019

Söderlind, Per; Landa, A.; Sadigh, B.
Advances in Physics, Vol. 68, Issue 1
DOI: 10.1080/00018732.2019.1599554

Assessing Relativistic Effects and Electron Correlation in the Actinide Metals Th to Pu
journal, November 2019

Sadigh, Babak; Kutepov, Andrey; Landa, Alexander
Applied Sciences, Vol. 9, Issue 23
DOI: 10.3390/app9235020

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

Kresse, G.; Furthmüller, J.
Physical Review B, Vol. 54, Issue 16, p. 11169-11186
DOI: 10.1103/PhysRevB.54.11169

Density of liquid uranium
journal, March 1970

Rohr, William G.; Wittenberg, Layton J.
The Journal of Physical Chemistry, Vol. 74, Issue 5
DOI: 10.1021/j100700a035

Features of cubic and tetragonal structures of U–Mo alloys: Atomistic simulation
journal, March 2016

Starikov, S. V.; Kolotova, L. N.
Scripta Materialia, Vol. 113
DOI: 10.1016/j.scriptamat.2015.10.012

Atomistic calculations of the surface energy as a function of composition and temperature in $γ$ U–Zr to inform fuel performance modeling
journal, November 2020

Beeler, Benjamin; Casagranda, Albert; Aagesen, Larry
Journal of Nuclear Materials, Vol. 540
DOI: 10.1016/j.jnucmat.2020.152271

Full-Potential Electronic Structure Method
book, January 2010

Wills, John M.; Eriksson, Olle; Andersson, Per
Springer Berlin, Heidelberg
DOI: 10.1007/978-3-642-15144-6

Evaluation of first-principles techniques for obtaining materials parameters of $α$ -uranium and the (001) $α$ -uranium surface
journal, March 2008

Taylor, Christopher D.
Physical Review B, Vol. 77, Issue 9
DOI: 10.1103/PhysRevB.77.094119

First-Principles Study of Properties of Alpha Uranium Crystal and Seven Alpha Uranium Surfaces
journal, January 2017

Huang, Shan-Qisong; Ju, Xue-Hai
Journal of Chemistry, Vol. 2017
DOI: 10.1155/2017/8618340

High-Temperature Heat Contents of Uranium, Uranium Dioxide and Uranium Trioxide ¹
journal, September 1947

Moore, G. E.; Kelley, K. K.
Journal of the American Chemical Society, Vol. 69, Issue 9
DOI: 10.1021/ja01201a009

Metallic fast reactor fuels
journal, January 1997

Hofman, G. L.; Walters, L. C.; Bauer, T. H.
Progress in Nuclear Energy, Vol. 31, Issue 1-2
DOI: 10.1016/0149-1970(96)00005-4

New interatomic potential for computation of mechanical and thermodynamic properties of uranium in a wide range of pressures and temperatures
journal, February 2012

Smirnova, D. E.; Starikov, S. V.; Stegailov, V. V.
The Physics of Metals and Metallography, Vol. 113, Issue 2
DOI: 10.1134/S0031918X12020147

Thermodynamics of Plutonium Monocarbide from Anharmonic and Relativistic Theory
journal, September 2020

Söderlind, Per; Landa, Alexander; Perron, Aurélien
Applied Sciences, Vol. 10, Issue 18
DOI: 10.3390/app10186524

Understanding thermally-activated glide of $1 / 2 〈 110 〉 {110}$ screw dislocations in UO2 – A molecular dynamics analysis
journal, November 2018

Lunev, A. V.; Starikov, S. V.; Aliev, T. N.
International Journal of Plasticity, Vol. 110
DOI: 10.1016/j.ijplas.2018.07.003

Lattice dynamics of $α$ uranium
journal, January 2008

Bouchet, J.
Physical Review B, Vol. 77, Issue 2
DOI: 10.1103/PhysRevB.77.024113

First-principles calculations of pure elements: Equations of state and elastic stiffness constants
journal, June 2010

Shang, S. L.; Saengdeejing, A.; Mei, Z. G.
Computational Materials Science, Vol. 48, Issue 4
DOI: 10.1016/j.commatsci.2010.03.041

The diffusion of point defects in uranium mononitride: Combination of DFT and atomistic simulation with novel potential
journal, February 2016

Kuksin, A. Yu.; Starikov, S. V.; Smirnova, D. E.
Journal of Alloys and Compounds, Vol. 658
DOI: 10.1016/j.jallcom.2015.10.223

Structural stability in uranium
journal, September 1997

Akella, J.; Weir, S.; Wills, J. M.
Journal of Physics: Condensed Matter, Vol. 9, Issue 39
DOI: 10.1088/0953-8984/9/39/003

Investigation of point defects diffusion in bcc uranium and U–Mo alloys
journal, March 2015

Smirnova, D. E.; Kuksin, A. Yu.; Starikov, S. V.
Journal of Nuclear Materials, Vol. 458
DOI: 10.1016/j.jnucmat.2014.12.080

Structure and Phase Transition Features of Monoclinic and Tetragonal Phases in U–Mo Alloys
journal, June 2020

Kolotova, Lada; Gordeev, Ilia
Crystals, Vol. 10, Issue 6
DOI: 10.3390/cryst10060515

First-principles study of diffusion of interstitial and vacancy in α U–Zr
journal, May 2011

Huang, Gui-Yang; Wirth, Brian D.
Journal of Physics: Condensed Matter, Vol. 23, Issue 20
DOI: 10.1088/0953-8984/23/20/205402

Projector augmented-wave pseudopotentials for uranium-based compounds
journal, January 2020

Torres, E.; Kaloni, T. P.
Computational Materials Science, Vol. 171
DOI: 10.1016/j.commatsci.2019.109237

Thermodynamic stabilization of $γ − U - Mo$ alloys: Effect of Mo content and temperature
journal, May 2020

Castellano, Aloïs; Bottin, François; Dorado, Boris
Physical Review B, Vol. 101, Issue 18
DOI: 10.1103/PhysRevB.101.184111

Thermodynamics Modeling for Actinide Monocarbides and Mononitrides from First Principles
journal, January 2022

Söderlind, Per; Moore, Emily E.; Wu, Christine J.
Applied Sciences, Vol. 12, Issue 2
DOI: 10.3390/app12020728

Characterization of metallic fuel for minor actinides transmutation in fast reactor
journal, January 2017

Capriotti, L.; Brémier, S.; Inagaki, K.
Progress in Nuclear Energy, Vol. 94
DOI: 10.1016/j.pnucene.2016.04.004

Ground-State and Thermodynamical Properties of Uranium Mononitride from Anharmonic First-Principles Theory
journal, September 2019

Söderlind, Per; Landa, Alexander; Perron, Aurélien
Applied Sciences, Vol. 9, Issue 18
DOI: 10.3390/app9183914

Atomic Simulations of U-Mo under Irradiation: A New Angular Dependent Potential
journal, June 2021

Ouyang, Wenhong; Lai, Wensheng; Li, Jiahao
Metals, Vol. 11, Issue 7
DOI: 10.3390/met11071018

The Thermodynamic Properties of the f-Elements and Their Compounds. I. The Lanthanide and Actinide Metals
journal, December 2010

Konings, Rudy J. M.; Beneš, Ondrej
Journal of Physical and Chemical Reference Data, Vol. 39, Issue 4
DOI: 10.1063/1.3474238

Atomistic modeling of high temperature uranium–zirconium alloy structure and thermodynamics
journal, December 2015

Moore, A. P.; Beeler, B.; Deo, C.
Journal of Nuclear Materials, Vol. 467
DOI: 10.1016/j.jnucmat.2015.10.016

High-temperature and high-pressure phase transitions in uranium
journal, February 2017

Bouchet, J.; Bottin, F.
Physical Review B, Vol. 95, Issue 5
DOI: 10.1103/PhysRevB.95.054113

Low-temperature irradiation behavior of uranium–molybdenum alloy dispersion fuel
journal, August 2002

Meyer, M. K.; Hofman, G. L.; Hayes, S. L.
Journal of Nuclear Materials, Vol. 304, Issue 2-3
DOI: 10.1016/S0022-3115(02)00850-4

First principles calculations of the structure and elastic constants of α, β and γ uranium
journal, February 2013

Beeler, Benjamin; Deo, Chaitanya; Baskes, Michael
Journal of Nuclear Materials, Vol. 433, Issue 1-3
DOI: 10.1016/j.jnucmat.2012.09.019

Dynamic methods for investigating thermophysical properties of matter at very high temperatures and pressures
journal, April 1986

Gathers, G. R.
Reports on Progress in Physics, Vol. 49, Issue 4
DOI: 10.1088/0034-4885/49/4/001

Enthalpy of uranium to 1500 K by drop calorimetry
journal, July 1976

Marchidan, D. I.; Ciopec, M.
The Journal of Chemical Thermodynamics, Vol. 8, Issue 7
DOI: 10.1016/0021-9614(76)90021-5

Cold and hot uranium in DFT calculations: Investigation by the GTH pseudopotential, PAW, and APW + lo methods
journal, November 2021

Migdal, K.; Yanilkin, A.
Computational Materials Science, Vol. 199
DOI: 10.1016/j.commatsci.2021.110665

A unified picture of the crystal structures of metals
journal, April 1995

Söderlind, Per; Eriksson, Olle; Johansson, Börje
Nature, Vol. 374, Issue 6522
DOI: 10.1038/374524a0

Quantum molecular dynamics simulations of uranium at high pressure and temperature
journal, July 2008

Hood, Randolph Q.; Yang, L. H.; Moriarty, John A.
Physical Review B, Vol. 78, Issue 2
DOI: 10.1103/PhysRevB.78.024116

Anisotropy of the U–Mo alloy: Molecular-dynamics study
journal, May 2016

Kolotova, L. N.; Starikov, S. V.
The Physics of Metals and Metallography, Vol. 117, Issue 5
DOI: 10.1134/S0031918X16050100

The structures of uranium metal
journal, April 1949

Wilson, A. S.; Rundle, R. E.
Acta Crystallographica, Vol. 2, Issue 2
DOI: 10.1107/S0365110X4900028X

Migration of minor actinides and lanthanides in fast reactor metallic fuel
journal, July 2009

Kim, Yeon Soo; Hofman, G. L.; Yacout, A. M.
Journal of Nuclear Materials, Vol. 392, Issue 2
DOI: 10.1016/j.jnucmat.2009.03.043

Atomistic simulation of cubic and tetragonal phases of U-Mo alloy: Structure and thermodynamic properties
journal, February 2018

Starikov, S. V.; Kolotova, L. N.; Kuksin, A. Yu.
Journal of Nuclear Materials, Vol. 499
DOI: 10.1016/j.jnucmat.2017.11.047

Crystal-structure stabilities and electronic structure for the light actinides Th, Pa, and U
journal, June 1992

Wills, J. M.; Eriksson, Olle
Physical Review B, Vol. 45, Issue 24
DOI: 10.1103/PhysRevB.45.13879

Elastic properties of the light actinides at high pressure
journal, May 2011

Bouchet, J.; Albers, R. C.
Journal of Physics: Condensed Matter, Vol. 23, Issue 21
DOI: 10.1088/0953-8984/23/21/215402

Ab initio molecular dynamics investigation of γ-(U,Zr) structural and thermal properties as a function of temperature and composition
journal, April 2022

Aly, Ahmed; Beeler, Benjamin; Avramova, Maria
Journal of Nuclear Materials, Vol. 561
DOI: 10.1016/j.jnucmat.2022.153523

High-Temperature Thermodynamics Modeling of Graphite
journal, July 2022

Söderlind, Per; Landa, Alexander; Hood, Randolph Q.
Applied Sciences, Vol. 12, Issue 15
DOI: 10.3390/app12157556

Description of phase transitions through accumulation of point defects: UN, UO2 and UC
journal, November 2018

Starikov, S.; Korneva, M.
Journal of Nuclear Materials, Vol. 510
DOI: 10.1016/j.jnucmat.2018.08.025

Calculated thermal expansion of the actinide elements
journal, July 1991

S�derlind, P.; Johansson, B.; Yongming, L.
International Journal of Thermophysics, Vol. 12, Issue 4
DOI: 10.1007/BF00534216

Heat Content of Molten Uranium
journal, June 1964

Levinson, L. S.
The Journal of Chemical Physics, Vol. 40, Issue 12
DOI: 10.1063/1.1725055

Phase diagram of uranium at high pressures and temperatures
journal, May 1998

Yoo, Choong-Shik; Cynn, Hyunchae; Söderlind, Per
Physical Review B, Vol. 57, Issue 17
DOI: 10.1103/PhysRevB.57.10359

Multiscale Modeling of Uranium Mononitride: Point Defects Diffusion, Self-Diffusion, Phase Composition
journal, May 2017

Starikov, Sergey; Kuksin, Alexey; Smirnova, Daria
Defect and Diffusion Forum, Vol. 375
DOI: 10.4028/www.scientific.net/DDF.375.101

Mechanical and Thermal Properties for Uranium and U–6Nb Alloy from First-Principles Theory
journal, June 2021

Söderlind, Per; Yang, Lin H.; Landa, Alexander
Applied Sciences, Vol. 11, Issue 12
DOI: 10.3390/app11125643

Computational Thermodynamics
book, January 2007

Lukas, Hans; Fries, Suzana G.; Sundman, Bo
DOI: 10.1017/CBO9780511804137

Interatomic potential for uranium in a wide range of pressures and temperatures
journal, December 2011

Smirnova, D. E.; Starikov, S. V.; Stegailov, V. V.
Journal of Physics: Condensed Matter, Vol. 24, Issue 1
DOI: 10.1088/0953-8984/24/1/015702

First principles calculations for defects in U
journal, November 2010

Beeler, B.; Good, B.; Rashkeev, S.
Journal of Physics: Condensed Matter, Vol. 22, Issue 50
DOI: 10.1088/0953-8984/22/50/505703

The atomistic simulation of pressure-induced phase transition in uranium mononitride
journal, November 2015

Tseplyaev, V. I.; Starikov, S. V.
Journal of Physics: Conference Series, Vol. 653
DOI: 10.1088/1742-6596/653/1/012092

Determination of Thermal Expansion, Defect Formation Energy, and Defect-Induced Strain of α-U Via ab Initio Molecular Dynamics
journal, June 2021

Beeler, Benjamin; Mahbuba, Khadija; Wang, Yuhao
Frontiers in Materials, Vol. 8
DOI: 10.3389/fmats.2021.661387

Classical mean-field approach for thermodynamics: Ab initio thermophysical properties of cerium
journal, May 2000

Wang, Yi
Physical Review B, Vol. 61, Issue 18
DOI: 10.1103/PhysRevB.61.R11863

Features of structure and phase transitions in pure uranium and U–Mo alloys: atomistic simulation
journal, November 2016

Kolotova, L. N.; Kuksin, A. Yu; Smirnova, D. E.
Journal of Physics: Conference Series, Vol. 774
DOI: 10.1088/1742-6596/774/1/012036

THE HEAT CAPACITY AND THERMODYNAMIC FUNCTIONS OF URANIUM FROM 5 TO 350°K. ¹
journal, July 1960

Flotow, Howard E.; Lohr, Harold R.
The Journal of Physical Chemistry, Vol. 64, Issue 7
DOI: 10.1021/j100836a021

Plane-wave pseudopotential study of point defects in uranium dioxide
journal, August 2001

Crocombette, J. P.; Jollet, F.; Nga, L. Thien
Physical Review B, Vol. 64, Issue 10
DOI: 10.1103/PhysRevB.64.104107

An equation for the heat capacity of solids
journal, February 1987

Fei, Yingwei; Saxena, S. K.
Geochimica et Cosmochimica Acta, Vol. 51, Issue 2
DOI: 10.1016/0016-7037(87)90236-5

Thermal-Hydraulic Challenges in Fast Reactor Design
journal, July 2009

Todreas, Neil E.
Nuclear Technology, Vol. 167, Issue 1
DOI: 10.13182/NT09-A8857

Quantum mechanical calculations of uranium phases and niobium defects in γ-uranium
journal, March 2008

Xiang, Shikai; Huang, Hanchen; Hsiung, L. M.
Journal of Nuclear Materials, Vol. 375, Issue 1
DOI: 10.1016/j.jnucmat.2007.11.003

When magnetism can stabilize the crystal structure of metals
journal, December 2008

Soderlind, P.; Moore, K.
Scripta Materialia, Vol. 59, Issue 12
DOI: 10.1016/j.scriptamat.2008.08.031

Plane-wave pseudopotential study of the light actinides
journal, December 2002

Richard, Nicolas; Bernard, Stéphane; Jollet, François
Physical Review B, Vol. 66, Issue 23
DOI: 10.1103/PhysRevB.66.235112

Similar Records in DOE PAGES and OSTI.GOV collections:

Thermodynamics of Plutonium Monocarbide from Anharmonic and Relativistic Theory

Journal Article Söderlind, Per ; Landa, Alexander ; Perron, Aurélien ; ... - Applied Sciences

Thermodynamics of plutonium monocarbide is studied from first-principles theory that includes relativistic electronic structure and anharmonic lattice vibrations. Density-functional theory (DFT) is expanded to include orbital-orbital coupling in addition to the relativistic spin-orbit interaction for the electronic structure and it is combined with anharmonic, temperature dependent, lattice dynamics derived from the self-consistent ab initio lattice dynamics (SCAILD) method. The obtained thermodynamics are compared to results from simpler quasi-harmonic theory and experimental data. Formation enthalpy, specific heat, and Gibbs energy calculated from the anharmonic model are validated by direct comparison with a calculation of phase diagram (CALPHAD) assessment of PuC andmore »« less
https://doi.org/10.3390/app10186524

Full Text Available
Thermodynamics Modeling for Actinide Monocarbides and Mononitrides from First Principles

Journal Article Söderlind, Per ; Moore, Emily E. ; Wu, Christine J. - Applied Sciences

The high-temperature thermodynamical properties for the actinide monocarbides and mononitrides ThC, ThN, UC, UN, PuC, and PuN are calculated from first-principles electronic-structure theory. The electronic structure is modeled with density-functional theory (DFT) and is fully relativistic, including the spin-orbit interaction. Furthermore, the DFT is extended to account for orbital–orbital interactions, by means of a parameter-free orbital-polarization (OP) technique, that has proven to be essential for the 5f electrons in plutonium. Strong anharmonicity and the temperature dependence of the lattice vibrations are captured with the self-consistent ab initio lattice dynamics (SCAILD) method. The calculated free energies and heat capacities are comparedmore »« less
https://doi.org/10.3390/app12020728

Full Text Available
Ground-State and Thermodynamical Properties of Uranium Mononitride from Anharmonic First-Principles Theory

Journal Article Söderlind, Per ; Landa, Alexander ; Perron, Aurélien ; ... - Applied Sciences

We report on an advanced density-functional theory (DFT) approach for investigating the ground-state and thermodynamical properties of uranium mononitride (UN). The electronic structure for UN at zero temperature is obtained from DFT that utilizes the generalized gradient approximation (GGA) for the electron exchange and correlation functional and includes spin-orbit interaction and an extension with orbital polarization. Thermodynamical properties are computed within the quasi-harmonic approximation in the Debye–Grüneisen model while anharmonicity is captured in the self-consistent ab initio lattice dynamics (SCAILD) scheme. Anharmonic phonons have heretofore never been modeled from first-principles for UN but they turn out to be important. Themore »« less
Cited by 12
https://doi.org/10.3390/app9183914

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

Journal Article Söderlind, Per ; Landa, A. ; Yang, L. H. ; ... - Physical Review. B

Here, we present results from density functional theory (DFT) calculations of the lattice dynamics (phonons) and thermodynamics for δ-phase plutonium. The fully relativistic electronic structure is calculated assuming a three-dimensional noncollinear magnetic structure in conjunction with DFT and the general gradient approximation for the electron exchange and correlation interactions. The electronic-structure model is further enhanced by addressing strong orbital-orbital coupling via the conventional orbital-polarization (OP) scheme as has been successfully done for plutonium. The temperature dependence of the phonons is calculated within the self-consistent ab initio lattice dynamics approach. The obtained phonons compare very well with measurements although a modestmore »« less
https://doi.org/10.1103/physrevb.108.104112
High-Temperature Thermodynamics Modeling of Graphite

Journal Article Söderlind, Per ; Landa, Alexander ; Hood, Randolph Q. ; ... - Applied Sciences

We present high-temperature thermodynamic properties for graphite from first-principles anharmonic theory. The ab initio electronic structure is obtained from density-functional theory coupled to a lattice dynamics method that is used to model anharmonic lattice vibrations. This combined approach produces free energies and specific heats for graphite that compare well with available experiments and results from models that empirically represent experimental data, such as CALPHAD. We show that anharmonic theory for the phonons is essential for accurate thermodynamic quantities above about 1000 K.
https://doi.org/10.3390/app12157556

Full Text Available

Similar Records

Title: High-Temperature Thermodynamics of Uranium from Ab Initio Modeling

Abstract

Citation Formats

Metallic fuels for advanced reactors journal, July 2009

Molecular-dynamic simulation of the thermophysical properties of liquid uranium journal, June 2010

A ternary EAM interatomic potential for U–Mo alloys with xenon journal, March 2013

Atomistic simulation of defect formation and structure transitions in U-Mo alloys in swift heavy ion irradiation journal, November 2017

High-temperature phonon stabilization of γ -uranium from relativistic first-principles theory journal, February 2012

Entropy Driven Stabilization of Energetically Unstable Crystal Structures Explained from First Principles Theory journal, March 2008

The atomistic simulation of pressure-induced phase transition in uranium mononitride journal, November 2016

Orbital polarization in narrow-band systems: Application to volume collapses in light lanthanides journal, April 1990

From ultrasoft pseudopotentials to the projector augmented-wave method journal, January 1999

First-principles elastic and structural properties of uranium metal journal, August 2002

Atomistic properties of γ uranium journal, February 2012

SGTE data for pure elements journal, October 1991

Atomistic Simulation of the Fission-Fragment-Induced Formation of Defects in a Uranium–Molybdenum Alloy journal, July 2019

First-principles study of bubble nucleation and growth behaviors in α U–Zr journal, September 2012

Thermodynamic properties of α-uranium journal, November 2016

The Heat Capacities of Uranium, Uranium Trioxide, and Uranium Dioxide from 15°K to 300°K journal, April 1952

Spin disorder in paramagnetic fcc iron journal, June 1989

First-principles phase stability, bonding, and electronic structure of actinide metals journal, June 2014

Understanding the Complex Phase Diagram of Uranium: The Role of Electron-Phonon Coupling journal, September 2011

Lattice dynamics simulation using machine learning interatomic potentials journal, February 2020

Elastic constants of cubic f -electron elements: Theory journal, October 1993

Thermo-Calc & DICTRA, computational tools for materials science journal, June 2002

Theory of the crystal structures of cerium and the light actinides journal, November 1998

Spin fluctuations in paramagnetic chromium determined from entropy considerations journal, June 1993

Thermal evolution of vibrational properties of α -U journal, November 2015

Heat capacity of metallic uranium and thorium from 80 to 1000 k journal, January 1980

Ab initio molecular dynamics investigation of point defects in γ -U journal, March 2021

Orbital polarization in the Kohn-Sham-Dirac theory journal, November 2005

Many-body interatomic U and Al–U potentials journal, May 2012

Atomistic modeling of the self-diffusion in γ-U and γ-U-Mo journal, May 2015

Density-functional theory for plutonium journal, January 2019

Assessing Relativistic Effects and Electron Correlation in the Actinide Metals Th to Pu journal, November 2019

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal, October 1996

Density of liquid uranium journal, March 1970

Features of cubic and tetragonal structures of U–Mo alloys: Atomistic simulation journal, March 2016

Atomistic calculations of the surface energy as a function of composition and temperature in γ U–Zr to inform fuel performance modeling journal, November 2020

Full-Potential Electronic Structure Method book, January 2010

Evaluation of first-principles techniques for obtaining materials parameters of α -uranium and the (001) α -uranium surface journal, March 2008

First-Principles Study of Properties of Alpha Uranium Crystal and Seven Alpha Uranium Surfaces journal, January 2017

High-Temperature Heat Contents of Uranium, Uranium Dioxide and Uranium Trioxide 1 journal, September 1947

Metallic fast reactor fuels journal, January 1997

New interatomic potential for computation of mechanical and thermodynamic properties of uranium in a wide range of pressures and temperatures journal, February 2012

Thermodynamics of Plutonium Monocarbide from Anharmonic and Relativistic Theory journal, September 2020

Understanding thermally-activated glide of 1 / 2 〈 110 〉 { 110 } screw dislocations in UO2 – A molecular dynamics analysis journal, November 2018

Lattice dynamics of α uranium journal, January 2008

First-principles calculations of pure elements: Equations of state and elastic stiffness constants journal, June 2010

The diffusion of point defects in uranium mononitride: Combination of DFT and atomistic simulation with novel potential journal, February 2016

Structural stability in uranium journal, September 1997

Investigation of point defects diffusion in bcc uranium and U–Mo alloys journal, March 2015

Structure and Phase Transition Features of Monoclinic and Tetragonal Phases in U–Mo Alloys journal, June 2020

First-principles study of diffusion of interstitial and vacancy in α U–Zr journal, May 2011

Projector augmented-wave pseudopotentials for uranium-based compounds journal, January 2020

Thermodynamic stabilization of γ − U − Mo alloys: Effect of Mo content and temperature journal, May 2020

Thermodynamics Modeling for Actinide Monocarbides and Mononitrides from First Principles journal, January 2022

Characterization of metallic fuel for minor actinides transmutation in fast reactor journal, January 2017

Ground-State and Thermodynamical Properties of Uranium Mononitride from Anharmonic First-Principles Theory journal, September 2019

Atomic Simulations of U-Mo under Irradiation: A New Angular Dependent Potential journal, June 2021

The Thermodynamic Properties of the f-Elements and Their Compounds. I. The Lanthanide and Actinide Metals journal, December 2010

Atomistic modeling of high temperature uranium–zirconium alloy structure and thermodynamics journal, December 2015

High-temperature and high-pressure phase transitions in uranium journal, February 2017

Low-temperature irradiation behavior of uranium–molybdenum alloy dispersion fuel journal, August 2002

First principles calculations of the structure and elastic constants of α, β and γ uranium journal, February 2013

Dynamic methods for investigating thermophysical properties of matter at very high temperatures and pressures journal, April 1986

Enthalpy of uranium to 1500 K by drop calorimetry journal, July 1976

Cold and hot uranium in DFT calculations: Investigation by the GTH pseudopotential, PAW, and APW + lo methods journal, November 2021

A unified picture of the crystal structures of metals journal, April 1995

Quantum molecular dynamics simulations of uranium at high pressure and temperature journal, July 2008

Anisotropy of the U–Mo alloy: Molecular-dynamics study journal, May 2016

The structures of uranium metal journal, April 1949

Migration of minor actinides and lanthanides in fast reactor metallic fuel journal, July 2009

Atomistic simulation of cubic and tetragonal phases of U-Mo alloy: Structure and thermodynamic properties journal, February 2018

Crystal-structure stabilities and electronic structure for the light actinides Th, Pa, and U journal, June 1992

Elastic properties of the light actinides at high pressure journal, May 2011

Ab initio molecular dynamics investigation of γ-(U,Zr) structural and thermal properties as a function of temperature and composition journal, April 2022

High-Temperature Thermodynamics Modeling of Graphite journal, July 2022

Description of phase transitions through accumulation of point defects: UN, UO2 and UC journal, November 2018

Calculated thermal expansion of the actinide elements journal, July 1991

Metallic fuels for advanced reactors
journal, July 2009

Molecular-dynamic simulation of the thermophysical properties of liquid uranium
journal, June 2010

A ternary EAM interatomic potential for U–Mo alloys with xenon
journal, March 2013

Atomistic simulation of defect formation and structure transitions in U-Mo alloys in swift heavy ion irradiation
journal, November 2017

High-temperature phonon stabilization of $γ$ -uranium from relativistic first-principles theory
journal, February 2012

Entropy Driven Stabilization of Energetically Unstable Crystal Structures Explained from First Principles Theory
journal, March 2008

The atomistic simulation of pressure-induced phase transition in uranium mononitride
journal, November 2016

Orbital polarization in narrow-band systems: Application to volume collapses in light lanthanides
journal, April 1990

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999

First-principles elastic and structural properties of uranium metal
journal, August 2002

Atomistic properties of γ uranium
journal, February 2012

SGTE data for pure elements
journal, October 1991

Atomistic Simulation of the Fission-Fragment-Induced Formation of Defects in a Uranium–Molybdenum Alloy
journal, July 2019

First-principles study of bubble nucleation and growth behaviors in α U–Zr
journal, September 2012

Thermodynamic properties of α-uranium
journal, November 2016

The Heat Capacities of Uranium, Uranium Trioxide, and Uranium Dioxide from 15°K to 300°K
journal, April 1952

Spin disorder in paramagnetic fcc iron
journal, June 1989

First-principles phase stability, bonding, and electronic structure of actinide metals
journal, June 2014

Understanding the Complex Phase Diagram of Uranium: The Role of Electron-Phonon Coupling
journal, September 2011

Lattice dynamics simulation using machine learning interatomic potentials
journal, February 2020

Elastic constants of cubic f -electron elements: Theory
journal, October 1993

Thermo-Calc & DICTRA, computational tools for materials science
journal, June 2002

Theory of the crystal structures of cerium and the light actinides
journal, November 1998

Spin fluctuations in paramagnetic chromium determined from entropy considerations
journal, June 1993

Thermal evolution of vibrational properties of $α$ -U
journal, November 2015

Heat capacity of metallic uranium and thorium from 80 to 1000 k
journal, January 1980

Ab initio molecular dynamics investigation of point defects in $γ$ -U
journal, March 2021

Orbital polarization in the Kohn-Sham-Dirac theory
journal, November 2005

Many-body interatomic U and Al–U potentials
journal, May 2012

Atomistic modeling of the self-diffusion in γ-U and γ-U-Mo
journal, May 2015

Density-functional theory for plutonium
journal, January 2019

Assessing Relativistic Effects and Electron Correlation in the Actinide Metals Th to Pu
journal, November 2019

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

Density of liquid uranium
journal, March 1970

Features of cubic and tetragonal structures of U–Mo alloys: Atomistic simulation
journal, March 2016

Atomistic calculations of the surface energy as a function of composition and temperature in $γ$ U–Zr to inform fuel performance modeling
journal, November 2020

Full-Potential Electronic Structure Method
book, January 2010

Evaluation of first-principles techniques for obtaining materials parameters of $α$ -uranium and the (001) $α$ -uranium surface
journal, March 2008

First-Principles Study of Properties of Alpha Uranium Crystal and Seven Alpha Uranium Surfaces
journal, January 2017

High-Temperature Heat Contents of Uranium, Uranium Dioxide and Uranium Trioxide ¹
journal, September 1947

Metallic fast reactor fuels
journal, January 1997

New interatomic potential for computation of mechanical and thermodynamic properties of uranium in a wide range of pressures and temperatures
journal, February 2012

Thermodynamics of Plutonium Monocarbide from Anharmonic and Relativistic Theory
journal, September 2020

Understanding thermally-activated glide of $1 / 2 〈 110 〉 {110}$ screw dislocations in UO2 – A molecular dynamics analysis
journal, November 2018

Lattice dynamics of $α$ uranium
journal, January 2008

First-principles calculations of pure elements: Equations of state and elastic stiffness constants
journal, June 2010

The diffusion of point defects in uranium mononitride: Combination of DFT and atomistic simulation with novel potential
journal, February 2016

Structural stability in uranium
journal, September 1997

Investigation of point defects diffusion in bcc uranium and U–Mo alloys
journal, March 2015

Structure and Phase Transition Features of Monoclinic and Tetragonal Phases in U–Mo Alloys
journal, June 2020

First-principles study of diffusion of interstitial and vacancy in α U–Zr
journal, May 2011

Projector augmented-wave pseudopotentials for uranium-based compounds
journal, January 2020

Thermodynamic stabilization of $γ − U - Mo$ alloys: Effect of Mo content and temperature
journal, May 2020

Thermodynamics Modeling for Actinide Monocarbides and Mononitrides from First Principles
journal, January 2022

Characterization of metallic fuel for minor actinides transmutation in fast reactor
journal, January 2017

Ground-State and Thermodynamical Properties of Uranium Mononitride from Anharmonic First-Principles Theory
journal, September 2019

Atomic Simulations of U-Mo under Irradiation: A New Angular Dependent Potential
journal, June 2021

The Thermodynamic Properties of the f-Elements and Their Compounds. I. The Lanthanide and Actinide Metals
journal, December 2010

Atomistic modeling of high temperature uranium–zirconium alloy structure and thermodynamics
journal, December 2015

High-temperature and high-pressure phase transitions in uranium
journal, February 2017

Low-temperature irradiation behavior of uranium–molybdenum alloy dispersion fuel
journal, August 2002

First principles calculations of the structure and elastic constants of α, β and γ uranium
journal, February 2013

Dynamic methods for investigating thermophysical properties of matter at very high temperatures and pressures
journal, April 1986

Enthalpy of uranium to 1500 K by drop calorimetry
journal, July 1976

Cold and hot uranium in DFT calculations: Investigation by the GTH pseudopotential, PAW, and APW + lo methods
journal, November 2021

A unified picture of the crystal structures of metals
journal, April 1995

Quantum molecular dynamics simulations of uranium at high pressure and temperature
journal, July 2008

Anisotropy of the U–Mo alloy: Molecular-dynamics study
journal, May 2016

The structures of uranium metal
journal, April 1949

Migration of minor actinides and lanthanides in fast reactor metallic fuel
journal, July 2009

Atomistic simulation of cubic and tetragonal phases of U-Mo alloy: Structure and thermodynamic properties
journal, February 2018

Crystal-structure stabilities and electronic structure for the light actinides Th, Pa, and U
journal, June 1992

Elastic properties of the light actinides at high pressure
journal, May 2011

Ab initio molecular dynamics investigation of γ-(U,Zr) structural and thermal properties as a function of temperature and composition
journal, April 2022

High-Temperature Thermodynamics Modeling of Graphite
journal, July 2022

Description of phase transitions through accumulation of point defects: UN, UO2 and UC
journal, November 2018

Calculated thermal expansion of the actinide elements
journal, July 1991

Heat Content of Molten Uranium
journal, June 1964

Phase diagram of uranium at high pressures and temperatures
journal, May 1998

Multiscale Modeling of Uranium Mononitride: Point Defects Diffusion, Self-Diffusion, Phase Composition
journal, May 2017