J. Phys. Soc. Jpn. 75S (2006) pp. 130-136  |Previous Article| |Next Article|  |Table of Contents|
|Full Text PDF: FREE (880K)|

Proc. of 5th Int. Symposium on ASR-WYP-2005 – Advances in the Physics and Chemistry of Actinide Compounds –

Probing the Bonding and Electronic Nature of Actinides Using Pressure

R. G. Haire

An important issue in actinide science is the changing role of the 5f electrons, both when progressing from element to element across the series and how experimental variables affect their roles in the elements' chemistries and physics. It has been established that the function of these 5f electrons can often be changed by experimental conditions. For instance, we have found that the 5f electrons of several actinide metals, their alloys and compounds are affected greatly by pressure, due to the very large decreases in interatomic distances that can occur. The latter bring about significant changes in the energy levels, and the potential for overlap or hybridization of electronic orbitals. These changes in electronic behavior and configuration for the f-elements for crystalline solids under pressure can be monitored via X-ray diffraction using correlations established between bonding and the structure exhibited. Evaluation of these changes provides unique insights into the bonding behavior of the f-elements. In contrast to the elements, observed structural changes with pressure with compounds may not be linked directly to the involvement of 5f electrons. For compounds, this is due in part to the presence and bonding role of non-actinide atoms, which affect both interatomic distances as well as the type of electronic orbitals that can interact. Some recent experimental findings together with results from theoretical computations allow important new insights to be gained into changes in electronic configurations and bonding for the actinide elements under pressure. These findings also afford correlations with regard to the elements' positions in the 5f series. The impact, present electronic interpretations and the implications of the data from these studies are discussed here, both from a standpoint of experimental studies and the theoretical work that have been done. In addition, some potential future thrusts in high-pressure research for additional insight into 5f electron science are also discussed.

URL: http://jpsj.ipap.jp/link?JPSJS/75S/130/
DOI: 10.1143/JPSJS.75S.130

References

1. M. S. S. Brooks, B. Johansson and H. L. Skriver: in Handbook on the Physics and Chemistry of the Actinides, ed. A. J. Freeman and G. H. Lander (North-Holland, Amsterdam, 1984) Vol. I, pp. 153–269.
2. R. G. Haire, S. Heathman, T. Le Bihan, A. Lindbaum and M. Iridi: in Investigations of Actinide Metals and Compounds under Pressure Provide Important Insights into Bonding and Chemistry, in MRS Symp. Proc., ed. L. Soderholm, J. J. Joyce, M. F. Nicol, D. K. Shuh and J. G. Tobin, eds., (MRS, Warrendale, PA, 2004) Vol. 802, pp. 15–21.
3. S. Heathman, R. G. Haire, T. Le Bihan, A. Lindbaun, K. Litfin, Y. Méresse and H. Libotte: Phys. Rev. Lett. 85 (2000) 2961[APS].
4. A. Lindbaum, S. Heathman, K. Litfin and Y. Méresse and R. G. Haire: Phys. Rev. B 63 (2001) 214101[APS].
5. T. Le Bihan, R. G. Haire, S. Heathman, M. Idiri and A. Lindbaum: J. Nucl. Sci. Technol. 3 (2002) Suppl., p. 45.
6. A. Lindbaum, S. Heathman, T. Le Bihan, R. G. Haire, M. Idiri and G. H. Lander: J. Phys.: Condens. Matter 15 (2003) S2297[IoP STACKS].
7. R. G. Haire, S. Heathman, M. Idiri, T. Le Bihan, A. Lindbaum and J. Rebizant: Phys. Rev. B 67 (2003) 134101[APS].
8. S. Heathman, R. G. Haire, T. Le Bihan, A. Lindbaum, M. Idiri, P. Normile, S. Li, R. Ahuja, B. Johansson and G. H. Lander: Science 309 (2005) 110[Science].
9. R. G. Haire, S. Heathman, T. Le Bihan and A. Lindbaum: NEA Publication, ISBN 92-64-18485-6 (2002) p. 147.
10. P. Söderlind and A. Landa: Phys. Rev. B 72 (2005) 024109[APS].
11. M. Pénicaud: J. Phys.: Condens. Matter 17 (2005) 257[IoP STACKS].
12. P. Söderlind, R. Ahuja, O. Eriksson, B. Johansson and J. M. Wills: Phys. Rev. B 61 (2000) 8119[APS].
13. R. G. Haire: Properties of the Transplutonium Metals (Am-Fm) in Metals Handbook (ASM International, Materials Park, Ohio, 1990) 10th ed., Vol. 2, pp. 1198–1201.
14. P. Söderlind: Europhys. Lett. 55 (2001) 525[CrossRef].
15. P. Söderlind, A. Landa and B. Sidigh: Phys. Rev. B 66 (2002) 205109[APS].
16. B. Sidigh, P. Söderlind and W. G. Wolfer: Phys. Rev. B 68 (2003) 241101R[APS].
17. A. L. Kutepov and S. G. Kutepova: J. Phys.: Condens. Matter 15 (2003) 260[IoP STACKS].
18. A. Landa and P. Söderlind: J. Alloys Compd. 354 (2003) 99.
19. A. M. Niklasson, J. M. Wills, M. I. Katsnelson, I. A. Abrikosov, O. Eriksson and B. Johansson: Phys. Rev. B 67 (2003) 235105[APS].
20. P. Söderlind and B. Sadigh: Phys. Rev. Lett. 92 (2004) 185702[APS].
21. J. Lashley, A. Lawson, R. J. McQueeney and G. H. Lander: Phys. Rev. B 72 (2005) 05416[APS].
22. R. G. Haire, U. Benedict, J. R. Peterson, C. Dufour and S. Dabos: Physica B+C 144 (1986) 19[CrossRef].
23. P. Söderlind, O. Eriksson, B. Johansson, J. M. Wills and A. M. Boring: Nature 374 (1995) 524[CrossRef].
24. O. K. Anderson, J. Madsen, U. K. Poulsen, O. Jepsen and J. Kollar: Physica B+C 86–88 (1977) 249[CrossRef].
25. P. Söderlind, R. Ahuja, O. Eriksson, J. M. Wills and B. Johansson: Phys. Rev. B 50 (1994) 5918[APS].
26. P. Link, D. Braithwaite, J. Wittig, U. Benedict and R. G. Haire: J. Alloys Compd. 213–214 (1994) 148.
27. J.-C. Griveau, J. Rebizant, G. H. Lander and G. Kotliar: Phys. Rev. Lett. 94 (2005) 097002[APS].
28. J. L. Smith and R. G. Haire: Science 200 (1978) 535
29. P. Söderlind and O. Eriksson: Phys. Rev. B 56 (1997) 10719[APS].