Thermodynamics Modeling for Actinide Monocarbides and Mononitrides from First Principles

Söderlind, Per; Moore, Emily E.; Wu, Christine J.

doi:10.3390/app12020728

Title: Thermodynamics Modeling for Actinide Monocarbides and Mononitrides from First Principles

Abstract

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 compared to published results from quasi-harmonic (QH) theory, and experiments, where available. For the uranium and plutonium compounds, we make use of CALPHAD assessments to help evaluate the theory. Generally, our anharmonic relativistic approach compares well with both CALPHAD and experiments. For the thorium compounds, our theory is in good accord with QH modeling of the free energy at lower temperatures but for the heat capacity the comparison is less favorable.

Authors:

^[1];

^[1]; Wu, Christine J. ^[1]

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

Publication Date:: Wed Jan 12 00:00:00 EST 2022

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

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

OSTI Identifier:: 1845635

Report Number(s):: LLNL-JRNL-829554
Journal ID: ISSN 2076-3417; 1045461; TRN: US2302460

Grant/Contract Number:: AC52-07NA27344

Resource Type:: Accepted Manuscript

Journal Name:: Applied Sciences

Additional Journal Information:: Journal Volume: 12; Journal Issue: 2; Journal ID: ISSN 2076-3417

Publisher:: MDPI

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; actinide monocarbides; mononitrides; free energy; specific heat; thermodynamics; anharmonic

Citation Formats


                    Söderlind, Per, Moore, Emily E., and Wu, Christine J. Thermodynamics Modeling for Actinide Monocarbides and Mononitrides from First Principles.  United States: N. p., 2022. 
Web.  doi:10.3390/app12020728.

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                    Söderlind, Per, Moore, Emily E., & Wu, Christine J. Thermodynamics Modeling for Actinide Monocarbides and Mononitrides from First Principles.  United States.  https://doi.org/10.3390/app12020728

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                    Söderlind, Per, Moore, Emily E., and Wu, Christine J. Wed .  
"Thermodynamics Modeling for Actinide Monocarbides and Mononitrides from First Principles".  United States.  https://doi.org/10.3390/app12020728.  https://www.osti.gov/servlets/purl/1845635.

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@article{osti_1845635,

  title        = {Thermodynamics Modeling for Actinide Monocarbides and Mononitrides from First Principles},

  author       = {Söderlind, Per and Moore, Emily E. and Wu, Christine J.},

  abstractNote = {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 compared to published results from quasi-harmonic (QH) theory, and experiments, where available. For the uranium and plutonium compounds, we make use of CALPHAD assessments to help evaluate the theory. Generally, our anharmonic relativistic approach compares well with both CALPHAD and experiments. For the thorium compounds, our theory is in good accord with QH modeling of the free energy at lower temperatures but for the heat capacity the comparison is less favorable.},

  doi          = {10.3390/app12020728},

  journal      = {Applied Sciences},

  number       = 2,

  volume       = 12,

  place        = {United States},

  year         = {Wed Jan 12 00:00:00 EST 2022},

  month        = {Wed Jan 12 00:00:00 EST 2022}

}

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Title: Thermodynamics Modeling for Actinide Monocarbides and Mononitrides from First Principles

Abstract

Citation Formats

Thermal Conductivity and Heat Capacity of the Monocarbide, Monophosphide, and Monosulfide of Uranium journal, July 1967

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

Projector augmented-wave method journal, December 1994

The Pu–U–Am system: An ab initio informed CALPHAD thermodynamic study journal, March 2015

Phase transformations in Pu–Ga alloy: Synergy between simulations and experiments to elucidate direct and indirect reversion competition journal, November 2013

Ab-initio investigations on dynamical and lattice thermal behaviours of ThC journal, April 2021

Structural stability and equation of state of thorium carbide for pressures up to 36 GPa journal, October 1986

Development of a CALPHAD Thermodynamic Database for Pu-U-Fe-Ga Alloys journal, November 2019

The influence of carbon non-stoichiometry on the electronic properties of thorium monocarbide ThC journal, September 2010

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

First principles investigation of thermal properties of thorium mononitride journal, October 2021

Thermodynamic modelling of advanced oxide and carbide nuclear fuels: Description of the U–Pu–O–C systems journal, December 2011

Uranium nitride as LWR TRISO fuel: Thermodynamic modeling of U–C–N journal, August 2012

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

Heat Capacity of Neptunium Mononitride journal, November 2002

Thermodynamical stability of substoichiometric plutonium monocarbide from first-principles calculations journal, January 2020

The self-consistent ab initio lattice dynamical method journal, January 2009

Thermodynamic modelling of the N–U system journal, July 2000

A new high-pressure phase of uranium nitride studied by X-ray diffraction and synchrotron radiation journal, February 1985

Crystallographic and magnetic ordering studies of plutonium carbides using neutron diffraction journal, March 1970

The chemical thermodynamic properties of nuclear materials journal, January 1973

Heat Capacity of Thorium Nitrides from 450 to 850K journal, July 1973

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

Spin disorder in paramagnetic fcc iron journal, June 1989

Generation-IV nuclear power: A review of the state of the science journal, December 2008

Effect of spin-orbit and on-site Coulomb interactions on the electronic structure and lattice dynamics of uranium monocarbide journal, August 2016

Phonon and magnetic structure in δ-plutonium from density-functional theory journal, October 2015

Chaleur specifique de UC et UN journal, January 1970

Is Hund's Second Rule Responsible for the Orbital Magnetism in Solids? journal, June 1998

Uranium mononitride: Heat capacity and thermal conductivity from 298 to 1000 °K journal, March 1971

Uranium Mononitride: Heat Capacity and Thermodynamic Properties from 5° to 350°K journal, July 1966

Exploring the sub-stoichiometric behavior of plutonium mononitride journal, January 2020

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

The heat capacity of uranium mononitride journal, February 1972

Heat Capacity of Plutonium Monocarbide from 400° to 1300°K journal, June 1964

A Consistent Set of Thermodynamic Values for Plutonium Mononitride journal, December 1968

A Screened Hybrid DFT Study of Actinide Oxides, Nitrides, and Carbides journal, June 2013

239PuN powder neutron diffraction study journal, October 1984

Phase stabilities and mechanical properties of two new carbon crystals journal, September 2009

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

Density-functional theory for plutonium journal, January 2019

Chaleur specifique de 2 a 300 K du monocarbure de thorium journal, September 1975

A molecular dynamics study of thorium nitride journal, May 2005

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

The chemical thermodynamic properties of nuclear materials I. Uranium mononitride journal, March 1972

First-principles investigation of uranium mononitride (UN): Effect of magnetic ordering, spin-orbit interactions and exchange correlation functional journal, February 2022

An investigation of the magnetic structure of uranium nitride by neutron diffraction journal, December 1965

A first principle calculation on electronic properties of plutonium mononitride: Insights from dynamical mean field theory journal, December 2018

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

Thermodynamic re-assessment of the Pu–U system and its application to the ternary Pu–U–Ga system journal, November 2014

The chemical thermodynamics of nuclear materials journal, February 1980

Thermophysical properties of thorium mononitride from 298 to 1700 K journal, December 2019

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

Phase transformations in PuGa 1at.% alloy: Study of whole reversion process following martensitic transformation journal, December 2013

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

Electronic structures, mechanical and thermodynamic properties of ThN from first-principles calculations journal, January 2011

First-principles study of point defects in thorium carbide journal, November 2014

Molecular dynamics studies of actinide nitrides journal, September 2005

The crystal structure and the equation of state of thorium nitride for pressures up to 47 GPa journal, October 1985

New Data on the Structure of Uranium Monocarbide journal, April 2008

Anomalous fcc Crystal Structure of Thorium Metal journal, July 1995

The chemical thermodynamic properties of nuclear materials III. Plutonium mononitride journal, October 1978

Lattice dynamics and thermal properties of thorium metal and thorium monocarbide journal, February 2020

Thermophysical Properties of Mixtures of Thorium and Uranium Nitride journal, September 2021

Thermal Conductivity and Heat Capacity of the Monocarbide, Monophosphide, and Monosulfide of Uranium
journal, July 1967

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

Projector augmented-wave method
journal, December 1994

The Pu–U–Am system: An ab initio informed CALPHAD thermodynamic study
journal, March 2015

Phase transformations in Pu–Ga alloy: Synergy between simulations and experiments to elucidate direct and indirect reversion competition
journal, November 2013

Ab-initio investigations on dynamical and lattice thermal behaviours of ThC
journal, April 2021

Structural stability and equation of state of thorium carbide for pressures up to 36 GPa
journal, October 1986

Development of a CALPHAD Thermodynamic Database for Pu-U-Fe-Ga Alloys
journal, November 2019

The influence of carbon non-stoichiometry on the electronic properties of thorium monocarbide ThC
journal, September 2010

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

First principles investigation of thermal properties of thorium mononitride
journal, October 2021

Thermodynamic modelling of advanced oxide and carbide nuclear fuels: Description of the U–Pu–O–C systems
journal, December 2011

Uranium nitride as LWR TRISO fuel: Thermodynamic modeling of U–C–N
journal, August 2012

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

Heat Capacity of Neptunium Mononitride
journal, November 2002

Thermodynamical stability of substoichiometric plutonium monocarbide from first-principles calculations
journal, January 2020

The self-consistent ab initio lattice dynamical method
journal, January 2009

Thermodynamic modelling of the N–U system
journal, July 2000

A new high-pressure phase of uranium nitride studied by X-ray diffraction and synchrotron radiation
journal, February 1985

Crystallographic and magnetic ordering studies of plutonium carbides using neutron diffraction
journal, March 1970

The chemical thermodynamic properties of nuclear materials
journal, January 1973

Heat Capacity of Thorium Nitrides from 450 to 850K
journal, July 1973

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

Spin disorder in paramagnetic fcc iron
journal, June 1989

Generation-IV nuclear power: A review of the state of the science
journal, December 2008

Effect of spin-orbit and on-site Coulomb interactions on the electronic structure and lattice dynamics of uranium monocarbide
journal, August 2016

Phonon and magnetic structure in δ-plutonium from density-functional theory
journal, October 2015

Chaleur specifique de UC et UN
journal, January 1970

Is Hund's Second Rule Responsible for the Orbital Magnetism in Solids?
journal, June 1998

Uranium mononitride: Heat capacity and thermal conductivity from 298 to 1000 °K
journal, March 1971

Uranium Mononitride: Heat Capacity and Thermodynamic Properties from 5° to 350°K
journal, July 1966

Exploring the sub-stoichiometric behavior of plutonium mononitride
journal, January 2020

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

The heat capacity of uranium mononitride
journal, February 1972

Heat Capacity of Plutonium Monocarbide from 400° to 1300°K
journal, June 1964

A Consistent Set of Thermodynamic Values for Plutonium Mononitride
journal, December 1968

A Screened Hybrid DFT Study of Actinide Oxides, Nitrides, and Carbides
journal, June 2013

239PuN powder neutron diffraction study
journal, October 1984

Phase stabilities and mechanical properties of two new carbon crystals
journal, September 2009

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

Density-functional theory for plutonium
journal, January 2019

Chaleur specifique de 2 a 300 K du monocarbure de thorium
journal, September 1975

A molecular dynamics study of thorium nitride
journal, May 2005

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

The chemical thermodynamic properties of nuclear materials I. Uranium mononitride
journal, March 1972

First-principles investigation of uranium mononitride (UN): Effect of magnetic ordering, spin-orbit interactions and exchange correlation functional
journal, February 2022

An investigation of the magnetic structure of uranium nitride by neutron diffraction
journal, December 1965

A first principle calculation on electronic properties of plutonium mononitride: Insights from dynamical mean field theory
journal, December 2018

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

Thermodynamic re-assessment of the Pu–U system and its application to the ternary Pu–U–Ga system
journal, November 2014

The chemical thermodynamics of nuclear materials
journal, February 1980

Thermophysical properties of thorium mononitride from 298 to 1700 K
journal, December 2019

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

Phase transformations in PuGa 1at.% alloy: Study of whole reversion process following martensitic transformation
journal, December 2013

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

Electronic structures, mechanical and thermodynamic properties of ThN from first-principles calculations
journal, January 2011

First-principles study of point defects in thorium carbide
journal, November 2014

Molecular dynamics studies of actinide nitrides
journal, September 2005

The crystal structure and the equation of state of thorium nitride for pressures up to 47 GPa
journal, October 1985

New Data on the Structure of Uranium Monocarbide
journal, April 2008

Anomalous fcc Crystal Structure of Thorium Metal
journal, July 1995

The chemical thermodynamic properties of nuclear materials III. Plutonium mononitride
journal, October 1978

Lattice dynamics and thermal properties of thorium metal and thorium monocarbide
journal, February 2020

Thermophysical Properties of Mixtures of Thorium and Uranium Nitride
journal, September 2021