Abstract.
Ab initio total energy calculations within the framework of density functional theory have been performed for atomic hydrogen and oxygen chemisorption on the (0001) surface of double hexagonal packed americium using a full-potential all-electron linearized augmented plane wave plus local orbitals method. Chemisorption energies were optimized with respect to the distance of the adatom from the relaxed surface for three adsorption sites, namely top, bridge, and hollow hcp sites, the adlayer structure corresponding to coverage of a 0.25 monolayer in all cases. Chemisorption energies were computed at the scalar-relativistic level (no spin-orbit coupling NSOC) and at the fully relativistic level (with spin-orbit coupling SOC). The two-fold bridge adsorption site was found to be the most stable site for O at both the NSOC and SOC theoretical levels with chemisorption energies of 8.204 eV and 8.368 eV respectively, while the three-fold hollow hcp adsorption site was found to be the most stable site for H with chemisorption energies of 3.136 eV at the NSOC level and 3.217 eV at the SOC level. The respective distances of the H and O adatoms from the surface were found to be 1.196 Åand 1.164 Å. Overall our calculations indicate that chemisorption energies in cases with SOC are slightly more stable than the cases with NSOC in the 0.049–0.238 eV range. The work functions and net magnetic moments respectively increased and decreased in all cases compared with the corresponding quantities of bare dhcp Am (0001) surface. The partial charges inside the muffin-tins, difference charge density distributions, and the local density of states have been used to analyze the Am-adatom bond interactions in detail. The implications of chemisorption on Am 5f electron localization-delocalization are also discussed.
Similar content being viewed by others
References
J.J. Katz, G.T. Seaborg, L.R. Morss, The Chemistry of the Actinide Elements (Chapman and Hall, 1986); L.R. Morss, J. Fuger, Transuranium Elements: A Half Century (American Chemical Society, Washington D.C., 1992); L.R. Morss, N.M. Edelstein, J. Fuger, Chemistry of the Actinide Transactinide Elements, edited by J.J. Katz, Hon (Springer, New York, 2006)
Challenges in Plutonium Science, Vol. I and II, Los Alamos Science, 26 (2000)
R. Haire, S. Heathman, M. Idiri, T. Le Bihan, A. Lindbaum, Nuclear Materials Technology/Los Alamos National Laboratory, 3rd/4th quarter 2003, p. 23
Fifty Years with Transuranium Elements, Proceedings of the Robert A. Welch Foundation, October 22–23, 1990, Houston, Texas
J.L. Sarrao, A.J. Schwartz, M.R. Antonio, P.C. Burns, R.G. Haire, H. Nitsche, Actinides 2005-Basic Science, Applications, and Technology, Proceedings of the Materials Research Society 893, (2005); K.J.M. Blobaum, E.A. Chandler, L. Havela, M.B. Maple, M.P. Neu, Actinides 2006-Basic Science, Applications, and Technology, Proceedings of the Materials Research Society 986, (2006)
The Elements beyond Uranium, G.T. Seaborg, W.D. Loveland (John Wiley & Sons, Inc. 1990), p. 17
S. Heathman, R.G. Haire, T. Le Bihan, A. Lindbaum, K. Litfin, Y. Méresse, H. Libotte, Phys. Rev. Lett. 85, 2961 (2000)
G.H. Lander, J. Fuger, Endeavour 13, 8 (1989)
A.J. Freeman, D.D. Koelling, inThe Actinides: Electronic Structure and Related Properties, edited by A.J. Freeman, J.B. Darby, Jr. (Academic, New York, 1974)
B. Johansson, Phys. Rev. B 11, 2740 (1975)
H.L. Skriver, O.K. Andersen, B. Johansson, Phys. Rev. Lett. 41, 42 (1978)
J.R. Naegele, L. Manes, J.C. Spirlet, W. Müller, Phys. Rev. Lett. 52, 1834 (1984)
A. Lindbaum, S. Heathman, K. Litfin, Y. Méresse, R.G. Haire, T. Le Bihan, H. Libotte, Phy. Rev. B 63, 214101 (2001)
M. Pénicaud, J. Phys.: Condens. Matter 14, 3575 (2002); M. Pénicaud, J. Phys.: Condens. Matter 17, 257 (2005)
S.Y. Savrasov, K. Haule, G. Kotliar, Phys. Rev. Lett. 96, 036404 (2006)
P. Sõderlind, R. Ahuja, O. Eriksson, B. Johansson, J.M. Wills, Phys. Rev. B. 61, 8119 (2000); P. Sõderlind, A. Landa, Phys. Rev. B. 72, 024109 (2005)
P.G. Huray, S.E. Nave, R.G. Haire, J. Less-Com. Met. 93, 293 (1983)
T. Gouder, P.M. Oppeneer, F. Huber, F. Wastin, J. Rebizant, Phys. Rev. B 72, 115122 (2005); L.E. Cox, J.W. Ward, R.G. Haire, Phys. Rev. B 45, 13239 (1992)
O. Eriksson, J.M. Wills, Phys. Rev. B 45, 3198 (1992)
A.L. Kutepov, S.G. Kutepova, J. Magn. Magn. Mat. 272, e329 (2004)
A. Shick, L. Havela, J. Kolorenc, V. Drchal, T. Gouder, P. M. Oppeneer, Phys. Rev. B 73, 104415 (2006)
S.Y. Savrasov, G. Kotliar, E. Abrahams, Nature 410, 793 (2001); G. Kotliar, D. Vollhardt, Phys. Today 57, 53 (2004); X. Dai, S.Y. Savrasov, G. Kotliar, A. Migliori, H. Ledbetter, E. Abrahams, Science 300, 953 (2003)
B. Johansson, A. Rosengren, Phys. Rev. B 11, 2836 (1975)
J.L. Smith, R.G. Haire, Science 200, 535 (1978)
J.C. Griveau, J. Rebizant, G.H. Lander, G. Kotliar, Phys. Rev. Lett. 94, 097002 (2005)
D. Gao, A.K. Ray, Eur. Phys. J. B 50, 497 (2006); D. Gao, A.K. Ray, MRS Fall 2005 Symp. Proc. 893, 39 (2006); D. Gao, A.K. Ray, Surf. Sci. 600, 4941 (2006); D. Gao, A.K. Ray, Eur. Phys. J.B 55, 13 (2007), and references therein
R. Atta-Fynn, A.K. Ray, Physica B 392, 112 (2007); R. Atta-Fynn, A.K. Ray Phys, Rev. B 75, 195112 (2007), and references therein
P. Hohenberg, W. Kohn, Phys. Rev. 136, B864 (1964); W. Kohn, L.J. Sham, Phys. Rev. 140, A1133 (1965)
J.P. Perdew, K. Burke, M. Ernzerhof, Phys. Rev. Lett. 77, 3865 (1996)
P. Blaha, K. Schwarz, G.K.H. Madsen, D. Kvasnicka, J. Luitz, WIEN2k, An Augmented Plane Wave Plus Local Orbitals Program for Calculating Crystal properties (Vienna University of Technology, Austria, 2001)
D.D. Koelling, B.N. Harmon, J. Phys. C 10, 3107 (1977)
J. Kunes, P. Novak, R. Schmid, P. Blaha, K. Schwarz, Phys. Rev. B 64, 153102 (2001)
F.D. Murnaghan, Proc. Natl. Acad. Sci. USA 30, 244 (1944)
R.W.G. Wyckoff, Crystal Structures (Wiley, New York, 1963), Vol. 1
F. Wagner, Th. Laloyaux, M. Scheffler, Phys. Rev. B 57, 2102 (1998); J.L.F. Da Silva, C. Stampfl, M. Scheffler, Surf. Sci. 600, 703 (2006)
A. Kokalj, J. Mol. Graphics Modeling 17, 176 (1999); code available from http://www.xcrysden.org
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Dholabhai, P., Atta-Fynn, R. & Ray, A. A density functional study of atomic hydrogen and oxygen chemisorption on the relaxed (0001) surface of double hexagonal close packed americium. Eur. Phys. J. B 61, 261–270 (2008). https://doi.org/10.1140/epjb/e2008-00071-7
Received:
Published:
Issue Date:
DOI: https://doi.org/10.1140/epjb/e2008-00071-7