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Experimental Benchmarking of Pu Electronic Structure


The standard method to determine the band structure of a condensed phase material is to (1) obtain a single crystal with a well defined surface and (2) map the bands with angle resolved photoelectron spectroscopy (occupied or valence bands) and inverse photoelectron spectroscopy (unoccupied or conduction bands). Unfortunately, in the case of Pu, the single crystals of Pu are either nonexistent, very small and/or having poorly defined surfaces. Furthermore, effects such as electron correlation and a large spin-orbit splitting in the 5f states have further complicated the situation. Thus, we have embarked upon the utilization of unorthodox electron spectroscopies, to circumvent the problems caused by the absence of large single crystals of Pu with well-defined surfaces. Our approach includes the techniques of resonant photoelectron spectroscopy [1], x-ray absorption spectroscopy [1,2,3,4], electron energy loss spectroscopy [2,3,4], Fano Effect measurements [5], and Bremstrahlung Isochromat Spectroscopy [6], including the utilization of micro-focused beams to probe single-crystallite regions of polycrystalline Pu samples. [2,3,6]



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1. Tobin, J.G., Chung, B.W., Schulze, R. K., Terry, J., Farr, J. D., Shuh, D. K., Heinzelman, K., Rotenberg, E., Waddill, G.D., and Van der Laan, G., “Resonant Photoemission in f-electron Systems: Pu and Gd”, Phys. Rev. B 68, 1155109 (October 2003).
2. Moore, K.T., Wall, M.A., Schwartz, A.J., Chung, B.W., Shuh, D.K., Schulze, R.K., and Tobin, J.G., “The Failure of Russell-Saunders Coupling in the 5f States of Plutonium”, Phys. Rev. Lett. 90, 196404 (May 2003).
3. van der Laan, G., Moore, K.T., Tobin, J.G., Chung, B.W., Wall, M.A., and Schwartz, A.J.,,“Applicability of the spin-orbit sum rule for the actinide 5f states,” Phys. Rev. Lett. 93, 097401 (Aug 2004).
4. Tobin, J.G., Moore, K.T., Chung, B.W., Wall, M.A., Schwartz, A.J., van der Laan, G., and Kutepov, A.L., “Competition Between Delocalization and Spin-Orbit Splitting in the Actinide 5f States,” Phys. Rev. B 72, 085109 (2005).
5. Tobin, J.G., Morton, S.A., Chung, B.W., Yuand, S.W., Waddill, G.D., “Spin-Resolved Electronic Structure Studies of Non-Magnetic Systems: Possible Observation of the Fano Effect in Polycrystal Ce,” submitted to Physica B, Proceedings of SCES05, Vienna, Austria, July 2005.
6. Tobin, J.G., Butterfield, M.T., Teslich, N.E. Jr, Bliss, R.A., Wall, M.A., McMahan, A.K., Chung, B.W., Schwartz, A.J., “Using Nano-focussed Bremstrahlung Isochromat Spectroscopy (nBIS) to Determine the Unoccupied Electronic Structure of Pu,” submitted to the Royal Society of Chemistry, Proceedings of the Actinides 2005 Meeting, Manchester, UK, July 2005.
7. Chung, B.W., Schwartz, A.J., Ebbinghaus, B.B., Fluss, M.J., Haslam, J.J., Blobaum, K.J.M., and Tobin, J.G., “Spectroscopic Signature of Aging in δ-Pu(Ga),” submitted to Europhysics Letters; B.W. Chung et al, MRS Symp. Proc. 2006.
8. Soderlind, P. and Sadigh, B., Phys. Rev. Lett. 92, 185702 (2004).
9. Soderlind, P., Landa, A., and Sadigh, B., Phys Rev. B 66, 205109 (2002).
10. Sadigh, B., Soderlind, P. and Wolfer, W., Phys. Rev. B 68, 241101R (2003).
11. Kotliar, G. and Vollhardt, D., Physics Today 57, 53 2004.
12. Saravsov, S.Y., Kotliar, G. and Abrahams, E., Nature 410, 793 (2001).
13. Baer, Y. and Lang, J.K., Phys. Rev B 21, 2060 (1980).
14. Penicaud, M., J. Phys. Condensed Matter 9, 6341 (1990).
15. Fano, U., Phys. Rev. 178, 131 (1969); 184, 250 (1969).
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17. Yu, S.W., Komesu, T., Chung, B.W., Waddill, G.D., Morton, S.A., and Tobin, J.G., “Study of the f electron correlations in nonmagnetic Ce by means of spin resolved resonant photoemission,” to be submitted to Phys. Rev. B, 2005.


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Experimental Benchmarking of Pu Electronic Structure


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