Delocalization and occupancy effects of 5f orbitals in plutonium intermetallics using L3-edge resonant X-ray emission spectroscopy

被引：47

作者：

Booth, C. H. ^{[1
]}

Medling, S. A. ^{[1
]}

Jiang, Yu ^{[1
]}

Bauer, E. D. ^{[2
]}

Tobash, P. H. ^{[3
]}

Mitchell, J. N. ^{[3
]}

Veirs, D. K. ^{[4
]}

Wall, M. A. ^{[5
]}

Allen, P. G. ^{[5
]}

Kas, J. J. ^{[6
]}

Sokaras, D. ^{[7
]}

Nordlund, D. ^{[7
]}

Weng, T. -C. ^{[7
]}

机构：

[1] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA

[2] Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USA

[3] Los Alamos Natl Lab, Mat Sci & Technol Div, Los Alamos, NM 87545 USA

[4] Los Alamos Natl Lab, Mfg Engn & Technol Div, Los Alamos, NM 87545 USA

[5] Lawrence Livermore Natl Lab, Div Mat Sci & Technol, Livermore, CA 94550 USA

[6] Univ Washington, Dept Phys, Seattle, WA 98195 USA

[7] SLAC Natl Accelerator Lab, Stanford Synchrotron Radiat Lightsource, Menlo Pk, CA 94025 USA

来源：

JOURNAL OF ELECTRON SPECTROSCOPY AND RELATED PHENOMENA | 2014年 / 194卷

关键词：

Actinide alloys and materials; Superconductors; Heavy fermions; Plutonium; XANES; RXES; TRANSITION-METAL-COMPLEXES; TEMPERATURE-DEPENDENCE; DECAMETHYLYTTERBOCENE COMPLEXES; CRYSTAL STRUCTURE; EDGE SPECTRA; PRESSURE; BIPYRIDINES; SCATTERING; SPECIATION; EXPANSION;

D O I：

10.1016/j.elspec.2014.03.004

中图分类号：

O433 [光谱学];

学科分类号：

0703 ; 070302 ;

摘要：

Although actinide (An) L-3-edge X-ray absorption near-edge structure (XANES) spectroscopy has been very effective in determining An oxidation states in insulating, ionically bonded materials, such as in certain coordination compounds and mineral systems, the technique fails in systems featuring more delocalized 5f orbitals, especially in metals. Recently, actinide L-3-edge resonant X-ray emission spectroscopy (RXES) has been shown to be an effective alternative. This technique is further demonstrated here using a parameterized partial unoccupied density of states method to quantify both occupancy and delocalization of the 5f orbital in alpha-Pu, delta-Pu, PuCoGa5, PuCoIn5, and PuSb2. These new results, supported by FEFF calculations, highlight the effects of strong correlations on RXES spectra and the technique's ability to differentiate between f-orbital occupation and delocalization. (C) 2014 Elsevier B.V. All rights reserved.

引用

页码：57 / 65

页数：9

共 61 条

[1]

[Anonymous], 1969, UCRL50174 LAWR LIV N

[2] Localized 5f electrons in superconducting PuCoIn5: consequences for superconductivity in PuCoGa5 [J].

Bauer, E. D. ;

Altarawneh, M. M. ;

Tobash, P. H. ;

Gofryk, K. ;

Ayala-Valenzuela, O. E. ;

Mitchell, J. N. ;

McDonald, R. D. ;

Mielke, C. H. ;

Ronning, F. ;

Griveau, J-C ;

Colineau, E. ;

Eloirdi, R. ;

Caciuffo, R. ;

Scott, B. L. ;

Janka, O. ;

Kauzlarich, S. M. ;

Thompson, J. D. .

JOURNAL OF PHYSICS-CONDENSED MATTER, 2012, 24 (05)

[3] Anderson lattice behavior in Yb1-xLuxAl3 -: art. no. 125102 [J].

Bauer, ED ;

Booth, CH ;

Lawrence, JM ;

Hundley, MF ;

Sarrao, JL ;

Thompson, JD ;

Riseborough, PS ;

Ebihara, T .

PHYSICAL REVIEW B, 2004, 69 (12)

[4] SELF-CONSISTENT LARGE-N EXPANSION FOR NORMAL-STATE PROPERTIES OF DILUTE MAGNETIC-ALLOYS [J].

BICKERS, NE ;

COX, DL ;

WILKINS, JW .

PHYSICAL REVIEW B, 1987, 36 (04) :2036-2079

[5] Effects of pressure on thermal transport in plutonium oxide powder [J].

Bielenberg, Patricia A. ;

Prenger, F. Coyne ;

Veirs, D. Kirk ;

Jones, Gerard F. .

INTERNATIONAL JOURNAL OF HEAT AND MASS TRANSFER, 2006, 49 (17-18) :3229-3239

[6] Self-irradiation damage to the local structure of plutonium and plutonium intermetallics [J].

Booth, C. H. ;

Jiang, Yu ;

Medling, S. A. ;

Wang, D. L. ;

Costello, A. L. ;

Schwartz, D. S. ;

Mitchell, J. N. ;

Tobash, P. H. ;

Bauer, E. D. ;

McCall, S. K. ;

Wall, M. A. ;

Allen, P. G. .

JOURNAL OF APPLIED PHYSICS, 2013, 113 (09)

[7] Multiconfigurational nature of 5f orbitals in uranium and plutonium intermetallics [J].

Booth, C. H. ;

Jiang, Yu ;

Wang, D. L. ;

Mitchell, J. N. ;

Tobash, P. H. ;

Bauer, E. D. ;

Wall, M. A. ;

Allen, P. G. ;

Sokaras, D. ;

Nordlund, D. ;

Weng, T-C. ;

Torrez, M. A. ;

Sarrao, J. L. .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2012, 109 (26) :10205-10209

[8] Quantifying structural damage from self-irradiation in a plutonium superconductor [J].

Booth, C. H. ;

Bauer, E. D. ;

Daniel, M. ;

Wilson, R. E. ;

Mitchell, J. N. ;

Morales, L. A. ;

Sarrao, J. L. ;

Allen, P. G. .

PHYSICAL REVIEW B, 2007, 76 (06)

[9] Intermediate-Valence Tautomerism in Decamethylytterbocene Complexes of Methyl-Substituted Bipyridines [J].

Booth, Corwin H. ;

Kazhdan, Daniel ;

Werkema, Evan L. ;

Walter, Marc D. ;

Lukens, Wayne W. ;

Bauer, Eric D. ;

Hu, Yung-Jin ;

Maron, Laurent ;

Eisenstein, Odile ;

Head-Gordon, Martin ;

Andersen, Richard A. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2010, 132 (49) :17537-17549

[10] Decamethylytterbocene Complexes of Bipyridines and Diazabutadienes: Multiconfigurational Ground States and Open-Shell Singlet Formation [J].

Booth, Corwin H. ;

Walter, Marc D. ;

Kazhdan, Daniel ;

Hu, Yung-Jin ;

Lukens, Wayne W. ;

Bauer, Eric D. ;

Maron, Laurent ;

Eisenstein, Odile ;

Andersen, Richard A. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2009, 131 (18) :6480-6491

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