Skip to main content Accessibility help

Symmetry reduction of δ-plutonium: an electronic-structure effect

  • Kevin T. Moore (a1), Per Söderlind (a2), Adam J. Schwartz (a3) and David Laughlin (a4)


Using first-principles density-functional theory calculations, we show that the anomalously large anisotropy of δ-plutonium is a consequence of greatly varying bond-strengths between the 12 nearest neighbors. Employing the calculated bond strengths, we expand the tenants of classical crystallography by incorporating anisotropy of chemical bonds, which yields a structure with the monoclinic space group Cm for δ-plutonium rather than face-centered cubic Fm3m. The reduced space group for δ-plutonium enlightens why the ground state of the metal is monoclinic, why distortions of the metal are viable, and has considerable implications for the behavior of the material as it ages. These results illustrate how an expansion of classical crystallography that accounts for anisotropic electronic structure can explain complicated materials in a novel way.



Hide All
[1] Bloss, F.D.Crystallography and Crystal Chemistry,” (Holt, Rinehart, and Winston Inc. 1971).
[2] Albers, R.C., Nature 410, 759 (2001).
[3] Hecker, S.S., Metall. Mat. Trans. A 35, 2207 (2004).
[4] Skrivers, H.L., Andersen, O.K. and Johansson, B., Phys. Rev. Lett. 41, 42 (1978).
[5] Smith, J.L. and Kmetko, E.A., J Less Comm. Met. 90, 83 (1983).
[6] Savrasov, S.Y., Kotliar, G. and Abrahams, E., Nature 410, 793 (2001).
[7] Moore, K.T. et al. , Phys. Rev. Lett 90, 196404 (2003).
[8] van der Laan, G. et al. , Phys. Rev. Lett 93, 097401 (2004).
[9] Wong, J. et al. , Science 301, 10781080 (2003).
[10] Ledbetter, H.M. and Moment, R.L., Acta Metall. 24, 891 (1976).
[11] McQueeney, R. J. et al. , Phys. Rev. Lett. 92, 146401 (2004).
[12] Stedman, R. and Nilsson, G., Phys. Rev. 145, 492 (1966).
[13] Moore, K.T., Söderlind, P., Schwartz, A.J., Laughlin, D.E., submitted to Phys. Rev. Lett.
[14] Wills, J.M., Eriksson, O., Alouani, M. and Price, D.L., “Electronic Structure and Physical Properties of Solids,” Dreysse, H., editor. (Springer-Verlag, Berlin, 1998).
[15] Ahuja, R., Söderlind, P., Trygg, J., Melsen, J., Wills, J.M., Johansson, B. and Eriksson, O., Phys Rev B 50, 14690 (1994).
[16] Söderlind, P. Adv Phys 47, 959. (1998).
[17] Perdew, J.P, Chevary, J.A., Vosko, S.H., Jackson, K.A., Pederson, M.R. and Singh, D.J., Phys Rev B 46, 6671 (1992).
[18] Perdew, J.P., Burke, K. and Ernzerhof, M., Phys Rev. Lett. 87, 156401 (2001).
[19] Chadi, D.J. and Cohen, M.L., Phys Rev B 8, 5747 (1973).
[20] Laughlin, D.E., Willard, M.A. and McHenry, M.E., “Phase Transformations and Evolution in Materials,” 2000, edited by Turchi, P., Gonis, A. (The Minerals, Metals and Materials Society) pp. 121.
[21] Söderlind, P. et al. , Phys Rev. B 45, 12911 (1992).
[22] Söderlind, P. and Sadigh, B., Phys. Rev. Lett 92, 185702 (2004).
[23] Elliot, R.O. and Gschneidner, K.A. Jr U.S. Patent Office, no. 3,043,727 (1962).
[24] Zukas, E.G. et al. , in Proceedings of an International Conference on Solid→Solid Phase Transformations, edited by Aaronson, H.I. et al. (The Metallurgical Society of AIME, 1981).
[25] King, H.W., J Mater. Sci. 1, 79 (1966).
[26] Predel, B. and Gust, W., Mater. Sci. Eng. 10, 211 (1972).
[27] Lawson, A.C. et al. , Phil Mag. B 80, 1869 (2000).
[28] Lawson, A.C. et al. , Phil Mag. B 85, 2007 (2005).
[29] Zocco, T.G. et al. , Acta Metall. 38, 2275 (1990).
[30] Schwartz, A.J. et al. ., Phil. Mag. 85, 479 (2005).
[31] Dai, X. et al. , Science 300, 953 (2003).
[32] Robert, G., Pasturel, A., and Siberchicot, B., J Phys. Con. Mat. 15, 8377 (2003).
[33] Cox, L.E. et al. , Phys Rev. B 51, 751 (1995).
[34] Coppens, P., X-ray charge densities and chemical bonding (Oxford University Press, 1997).
[35] We have attempted detection of extra reflections using electron diffraction in a transmission electron microscope (TEM). However, high thermal diffuse scattering, large amounts of double diffraction due to the high atomic number, and omnipresent surface oxidation have precluded the ability to do this. For these reasons, x-ray diffraction of large, single-grain samples performed at low temperatures will be the appropriate experiment.



Full text views

Total number of HTML views: 0
Total number of PDF views: 0 *
Loading metrics...

Abstract views

Total abstract views: 0 *
Loading metrics...

* Views captured on Cambridge Core between <date>. This data will be updated every 24 hours.

Usage data cannot currently be displayed