Abstract
Hybrid density functional theory has been used to systematically study the electronic, geometric, and magnetic properties of strongly correlated materials PuO2±x , UO2±x , and U0.5Pu0.5O2±x with x = 0.25. The calculations have been performed using the all-electron full- potential linearized augmented plane wave plus local orbitals basis (FP-L/APW+lo) method. Each compound has been studied at the ferromagnetic (FM) and anti-ferromagnetic (AFM) configurations with and without spin-orbit coupling (SOC) and full geometry optimizations. The optimized lattice constants, bulk moduli, and band gaps are reported. Total energy calculations indicate that the ground states are AFM for all compounds studied here and the band gaps are typically higher than 1.0 eV, characteristic of semiconductors. The total energy is lowered significantly and the band gaps increase with the inclusion of SOC. The chemical bonds between the actinide metals and oxygen atoms are primarily ionic in character.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
References
Los Alamos Science, edited by N.G. Cooper (Los Alamos National Laboratory, Los Alamos, NM 2000), Vol. 26
F. Weigel, J.J. Katz, G.T. Seaborg, in The Chemistry of the Actinide Elements, edited by J.J. Katz, G.T. Seaborg, L.R. Morss (Chapman & Hall, New York, 1986), Vol. 1, p. 680
J.M. Haschke, T.H. Allen, L.A. Morales, Science 287, 285 (2000)
M. Idiri, T. Le Bihan, S. Heathman, J. Rebizant, Phys. Rev. B 70, 014113 (2004)
H.Y. Geng, Y. Chen, Y. Kaneta, M. Kinoshita, Phys. Rev. B 75, 054111 (2007)
H.Y. Geng, Y. Chen, Y. Kaneta, M. Iwasawa, T. Ohnuma, M. Kinoshita, Phys. Rev. B 77, 104120 (2008)
B.T.M. Willis, J. Chem. Soc., Faraday Trans. 2 83, 1073 (1987)
S.D. Conradson, D. Manara, F. Wastin, D.L. Clark, G.H. Lander, L.A. Morales, J. Rebizant, V.V. Rondinella, Inorg. Chem. 43, 6922 (2004)
D.A. Andersson, T. Watanabe, C. Deo, B.P. Uberuaga, Phys. Rev. B 80, R060101 (2009)
D.A. Andersson, J. Lezama, B.P. Uberuaga, C. Deo, S.D. Conradson, Phys. Rev. B 79, 024110 (2009)
B.T.M. Willis, Acta Crystallogr., Sect. A: Cryst. Phys., Diffr., Theor. Gen. Crystallogr. 34, 88 (1978)
D.J.M. Bevan, I.E. Grey, B.T.M. Willis, J. Solid State Chem. 61, 1 (1986)
Y. Sagayama, Proc. Global 2007 (Boise, Idaho, USA, 2007), p. 251
H. Funasaka, M. Ito, Proc. Global 2007 (Boise, Idaho, USA, 2007), p. 259
J.C. Boettger, A.K. Ray, Int. J. Quantum Chem. 80, 824 (2000)
X. Wu, A.K. Ray, Eur. Phys. J. B 19, 343 (2001)
K.N. Kudin, G.E. Scuseria, R.L. Martin, Phys. Rev. Lett. 89, 266402 (2003)
J. Schoenes, J. Appl. Phys. 49, 1463 (1978)
C.E. McNeilly, J. Nucl. Mater. 11, 53 (1964)
M. Butterfield, T. Durakiewicz, E. Guziewicz, J. Joyce, A. Arko, K. Graham, D. Moore, L. Morales, Surf. Sci. 571, 74 (2004)
J.P. Perdew, A. Zunger, Phys. Rev. B 23, 5048 (1981)
L. Petit, A. Svane, Z. Szotek, W. Temmerman, Science 301, 498 (2003)
A. Svane, L. Petit, Z. Szotek, W.M. Temmerman, Phys. Rev. B 76, 115116 (2007)
R. Atta-Fynn, A.K. Ray, Chem. Phys. Lett. 482, 223 (2009)
J. Wang, L. Ma, A.K. Ray, Phys. Lett. A 374, 4704 (2010)
K.N. Kudin, G.E. Scuseria, R.L. Martin, Phys. Rev. Lett. 89, 266402 (2002)
I.D. Prodan, G.E. Scuseria, J.A. Sordo, K.N. Kudin, R.L. Martin, J. Chem. Phys. 123, 014703 (2005)
R. Atta-Fynn, A.K. Ray, Europhys. Lett. 85, 27008 (2009)
F. Islam, A.K. Ray, Solid State Commun. 150 (2010) 938
B. Sun, P. Zhang, X.G. Zhao, J. Chem. Phys. 128, 084705 (2008)
G. Jomard, B. Amadon, F. Bottin, M. Torrent, Phys. Rev. B 78, 075125 (2008)
A. Georges, G. Kotliar, W. Krauth, M.J. Rozenberg, Rev. Mod. Phys. 68, 13 (1996)
S.Y. Savrasov, G. Kotliar, E. Abrahams, Nature (London) 793, 410 (2001)
L. Ma, R. Atta-Fynn, A.K. Ray, submitted for publication
J.P. Perdew, K. Burke, M. Ernzerhof, Phys. Rev. Lett. 77, 3865 (1996)
K. Schwarz, P. Blaha, G.K.H. Madsen, Comput. Phys. Commun. 147, 71 (2002)
P. Blaha, K. Schwarz, G.K.H. Madsen, D. Kvasnicka, J. Luitz, WIEN2K, An Augmented Plane Wave+Local Orbitals Program for Calculating Crystal Properties (Technische Universität Wien, Austria, 2001)
F. Tran, P. Blaha, K. Schwarz, Phys. Rev. B 74, 155108 (2006)
P.E. Blöchl, O. Jepsen, O.K. Andersen, Phys. Rev. B 49, 16223 (1994)
P. Blaha, K. Schwarz, P.I. Sorantin, S.B. Trickey, Comput. Phys. Commun. 59, 399 (1990)
M. Petersen, F. Wagner, L. Hufnagel, M. Scheffler, P. Blaha, K. Schwarz, Comput. Phys. Commun. 126, 294 (2000)
F.D. Murnaghan, Proc. Natl. Acad. Sci. USA 30, 244 (1944)
E.R. Gardner, T.L. Markin, R.S. Street, J. Inorg. Nucl. Chem. 27, 541 (1965)
L.R. Morss, L.R. in The Chemistry of the Actinide Elements, 2nd edn. (edited by J.J. Katz, G.T. Seaborg, L.R. Morss, Chapman and Hall, London, 1986), Vol. 2, pp. 1278–1360
P. Villars, L.D. Calvert, Pearson’s Handbook of Crystallographic Data for Intermetallic Phases, 2nd edn. (ASM International, Materials Park, Ohio, 1991)
J. Schoenes, J. Appl. Phys. 49, 1463 (1978)
P.A. Korzhavyi, L. Vitos, D.A. Andersson, B. Johansson, Nat. Mater. 3, 225 (2004)
L. Vegard, Die Konstitution der Mischkristalle und die Raumfüllung der Atome, Z. Physik 5, 17 (1921)
A.R. Denton, N.W. Ashcroft, Phys. Rev. A 43, 3161 (1991)
B. Dorado, G. Jomard, M. Freyss, M. Bertolus, Phys. Rev. B 82, 035114 (2010)
R. Laskowski, G.K.H. Madsen, P. Blaha, K. Schwarz, Phys. Rev. B 69, R140408 (2004)
D. Gao, A.K. Ray Phys. Rev. B 77, 035123 (2008)
R. Atta-Fynn, A.K. Ray, Phys. Rev. B 76, 115101 (2007)
M. Freyss, N. Vergnet, T. Petit, J. Nucl. Mater. 352, 144 (2006)
P. Martin, S. Grandjean, M. Ripert, M. Freyss, P. Blanc, T. Petit, J. Nucl. Mater. 320, 138 (2003)
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Ma, L., Ray, A.K. An ab initio study of PuO2±0.25, UO2±0.25, and U0.5Pu0.5O2±0.25 . Eur. Phys. J. B 81, 103–113 (2011). https://doi.org/10.1140/epjb/e2011-10759-0
Received:
Revised:
Published:
Issue Date:
DOI: https://doi.org/10.1140/epjb/e2011-10759-0