Abstract
In this study, the lattice dynamics and thermal characteristics of thorium dioxide are calculated using the first-principle calculations based on the density functional theory (DFT). The Gibbs free energy, isothermal bulk moduli, Debye temperature, thermal Grüneisen parameter as well as vibrational contributions of Helmholtz free energy, internal energy and entropy of thorium dioxide are studied for the first time under high temperatures and pressures. Thermal properties are compared using generalized gradient approximation (GGA) and local density approximation (LDA) under a novel model based on the quasi-harmonic Debye–Einstein method. The results of the simulation reveal that the lattice constant calculated by LDA is less than the one calculated by GGA, while the Gibbs free energy, Debye temperature, adiabatic and isothermal bulk modulus obtained from LDA are greater than ones obtained from GGA. The volumetric thermal expansion coefficient and vibrational contribution of entropy obtained from GGA and LDA increase with rise in temperature.
Similar content being viewed by others
References
Dorado B, Amadon B, Freyss M and Bertolus M 2009 Phys. Rev. B: Condens. Matter 79 235125
Herring J S, MacDonald P E, Weaver K D and Kullberg C 2001 Nucl. Eng. Des. 203 65
Park J, Farfán E B, Mitchell K, Resnick A, Enriquez C and Yee T 2018 J. Nucl. Mater. 504 198
Scott S M, Yao T, Lu F, Xin G, Zhu W and Lian J 2017 J. Nucl. Mater. 485 207
Todosow M, Galperin A, Herring S, Kazimi M, Downar T and Morozov A 2005 Nucl. Technol. 151 168
Cozzo C, Staicu D, Somers J, Fernandez A and Konings R 2011 J. Nucl. Mater. 416 135
Young R A 1979 J. Nucl. Mater. 87 283
Olander D 2009 J. Nucl. Mater. 389 1
Di Marcello V, Rondinella V, Schubert A, van de Laar J and Van Uffelen P 2014 Prog. Nucl. Energy 72 83
Carbajo J J, Yoder G L, Popov S G and Ivanov V K 2001 J. Nucl. Mater. 299 181
Fink J 2000 J. Nucl. Mater. 279 1
Abram T and Ion S 2008 Energy Policy 36 4323
Atta-Fynn R and Ray A K 2007 Phys. Rev. B: Condens. Matter 76 115101
Lim I S and Scuseria G E 2008 Chem. Phys. Lett. 460 137
Park J, Farfán E B and Enriquez C 2018 Nucl. Eng. Technol. 50 731
Pegg J T, Aparicio-Angles X, Storr M and de Leeuw N H 2017 J. Nucl. Mater. 492 269
Shields A E, Santos-Carballal D and de Leeuw N H 2016 J. Nucl. Mater. 473 99
Serizawa H, Arai Y and Suzuki Y 2000 J. Nucl. Mater. 280 99
Willis B 1963 Proc. R Soc. London A Math. Phys. Sci. 274 134
Olsen J S, Gerward L, Kanchana V and Vaitheeswaran G 2004 J. Alloys Compd. 381 37
Dancausse J-P, Gering E, Heathman S and Benedict U 1990 High Pressure Res. 2 381
Li S, Ahuja R and Johansson B 2002 High Pressure Res. 22 471
Yamashita T, Nitani N, Tsuji T and Inagaki H 1997 J. Nucl. Mater. 245 72
Belle J and Berman R 1984 Thorium dioxide: properties and nuclear applications, USDOE Assistant Secretary for Nuclear Energy, Washington, DC
Giannozzi P, Baroni S, Bonini N, Calandra M, Car R, Cavazzoni C et al 2009 J. Phys.: Condens. Matter 21 395502
Perdew J P, Burke K and Ernzerhof M 1996 Phys. Rev. Lett. 77 3865
Perdew J P and Zunger A 1981 Phys. Rev. B: Condens. Matter 23 5048
Pack J D and Monkhorst H J 1977 Phys. Rev. B: Condens. Matter 16 1748
Kulik H J, Cococcioni M, Scherlis D A and Marzari N 2006 Phys. Rev. Lett. 97 103001
Schlegel H B 1982 J. Comput. Chem. 3 214
Di Ventra M and Pantelides S T 2000 Phys. Rev. B: Condens. Matter 61 16207
Baroni S, De Gironcoli S, Dal Corso A and Giannozzi P 2001 Rev. Mod. Phys. 73 515
Baroni S, Giannozzi P and Isaev E 2010 Rev. Mineral. Geochem. 71 39
Otero-de-la-Roza A, Abbasi-Pérez D and Luaña V 2011 Comput. Phys. Commun. 182 2232
Bendaif S, Boumaza A, Nemiri O, Boubendira K, Meradji H, Ghemid S et al 2015 Bull. Mater. Sci. 38 365
Bouayed M, Yakoubi A, Ahmed R, Khachai H, Khenata R, Naqib S et al 2020 Bull. Mater. Sci. 43 1
Birch F 1978 J. Geophys. Res. Solid Earth 83 1257
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Sahafi, M.H., Mahdavi, M. Ab initio investigations on lattice dynamics and thermal characteristics of ThO2 using Debye–Einstein model. Bull Mater Sci 44, 96 (2021). https://doi.org/10.1007/s12034-021-02370-0
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s12034-021-02370-0