Abstract
Here, we demonstrate the power of electron energy-loss spectroscopy (EELS) in a transmission electron microscope (TEM) to investigate the electronic structure plutonium. Using EELS, TEM, and synchrotron-radiation-based X-ray absorption spectroscopy (XAS), we provide the first experimental evidence that Russell-Saunders (LS) coupling fails for the 5f states of Pu. These results support the assumption that only the use of jj or intermediate coupling is appropriate for the 5f states of Pu. EELS experiments were performed in a TEM and are coupled with image and diffraction data, therefore, the measurements are completely phase specific. It is shown that EELS in a TEM may be used to circumvent the difficulty of producing single-phase or single-crystal samples due to its high spatial resolution.
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References
R.C. Albers, Nature 410, 759 (2001).
S.Y. Savrasov, G. Kotliar, E. Abrahams, Nature 410, 793 (2001).
G. Lander, Science 301, 1057 (2003).
X. Dai et al., Science 300, 953 (2003).
J. Wong et al., Science 301, 1078 (2003).
J.L. Sarrao et al., Nature 420, 297 (2002).
I. Opahle, P.M. Oppeneer, Phys. Rev. Lett. 90, 157001 (2003).
T. Maehiro et al., Phys. Rev. Lett. 90, 207007 (2003).
S.S. Hecker, MRS Bulletin 26, 872 (2001) and reference therein.
S.Y. Savrasov and G. Kotliar, Phys. Rev. Lett. 84, 3670 (2000).
P. Söderlind, Europhys. Lett. 55, 525 (2001).
R. Eisberg and R. Resnick, “Quantum Physics,” John Wiley and Sons, NY, 1974
C. Kittel, “Introduction to Solid State Physics,” 5th Ed., John Wiley and Sons, NY, 1976, page 442.
H.L. Skrivers, O.K. Andersen, and B. Johansson, Phys. Rev. Lett. 41, 42 (1978).
Cooper et al. “Hybridization-induced anisotropy in cerium and actinide systems” in Handbook on the physics and chemistry of the actinides, ed. A.J. Freeman and G.H. Lander, Elsevier Science, Vol. 2, 1985.
R.F. Egerton, “Electron energy-loss spectroscopy in the electron microscope” 2nd Ed., Plenum Press, NY, 1996, page 221.
J.G. Tobin et al., Phys. Rev. B 68, 115109 (2003).
M. Aono et al., Solid State. Commun. 39, 1057 (1981).
M. Cukier et al., J. Phys. (Paris) 39, L315 (1978).
L. Havela et al., Phys. Rev. B 65, 235118 (2002).
“Electronic Structure of Solids: Photoemission Spectra and Related Data,” ed. A. Goldmann and E. Koch, Landolt-Bornstein Numerical Data and Functional Relationships in Science and Technology, Group III, Vol. 23, Springer-Verlag Berlin, Germany, 1994. For rare earths: Subvolume 23a, Chapter 2.5 by W.D. Schneider. For actinides: Subvolume 23b, Chapter 2.8 by J.R. Naegale.
J.L. Dehmer et al., Phys. Rev. Lett. 26, 1521 (1971).
A.F. Starace, Phys. Rev. B 5, 1773 (1972).
J. Sugar, Phys. Rev. B 5, 1785 (1972).
L.I. Johansson et al., Phys. Rev. B 21, 1408 (1980).
P. Söderlind, Thesis (Uppsala, 1994) page 83.
Y. Baer and J.K. Lang, Phys. Rev. B 21, 2060 (1980).
M. Pénicaud, J. Phys: Condens. Matter. 9, 6341 (1997).
Acknowledgments
This work was performed under the auspices of the United States Department of Energy by Lawrence Livermore National Laboratory under contract W-7405-Eng-48, with support from Lawrence Berkeley National Laboratory (Contract No. DE-AC03-76SF00098). The Advanced Light Source and the Spectromicroscopy Facility (Beamline 7.0) have been built and operated under funding from the Office of Basic Energy Science at Department of Energy. The authors wish to thank Gil Gallegos for Ce samples, Jason Lashley and Michael Blau for the Pu samples, and J. Terry, J.D. Farr, T. Zocco, K. Heinzelman, and E. Rotenberg for help with the Pu data collection at the Advanced Light Source.
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Moore, K.T., Wall, M.A., Schwartz, A.J. et al. Experimental verification of the need for either jj or intermediate coupling in the 5f states of plutonium. MRS Online Proceedings Library 802, 66–74 (2003). https://doi.org/10.1557/PROC-802-DD2.6
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DOI: https://doi.org/10.1557/PROC-802-DD2.6