Observation of 5f intermediate coupling in uranium x-ray emission spectroscopy

Tobin, J. G.; Nowak, S.; Yu, S-W; Alonso-Mori, R.; Kroll, T.; Nordlund, D.; Weng, T-C; Sokaras, D.

doi:10.1088/2399-6528/ab6940

Title: Observation of 5f intermediate coupling in uranium x-ray emission spectroscopy

Abstract

The first observation of Intermediate Coupling effects in the occupied 5f states has been made using X-ray Emission Spectroscopy (XES). In the past, the impact of Intermediate Coupling of the 5f states in actinides has long been observed and quantified, using X-ray Absorption Spectroscopy (XAS) to probe the unoccupied 5f states, providing great insight into the enigma of 5f electronic structure, but no measure of its effects in the occupied states had been reported. Moreover, because the 5f occupied states in UF4 are almost completely of 5f5/2 character, the observed effect in XES is twice that in XAS for UF4.

Authors:

; Nowak, S.; Yu, S-W; Alonso-Mori, R.; Kroll, T.; Nordlund, D.; Weng, T-C; Sokaras, D.

Publication Date:: Fri Jan 17 00:00:00 EST 2020

Research Org.:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office; USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR)

OSTI Identifier:: 1592176

Alternate Identifier(s):: OSTI ID: 1582452; OSTI ID: 1597210

Report Number(s):: LLNL-JRNL-787893
Journal ID: ISSN 2399-6528

Grant/Contract Number:: AC02-76SF00515; AC52-07NA27344; AC02-05CH11231

Resource Type:: Published Article

Journal Name:: Journal of Physics Communications

Additional Journal Information:: Journal Name: Journal of Physics Communications Journal Volume: 4 Journal Issue: 1; Journal ID: ISSN 2399-6528

Publisher:: IOP Publishing

Country of Publication:: United Kingdom

Language:: English

Subject:: 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 36 MATERIALS SCIENCE; x-ray emission; actinides; uranium; angular momentum coupling

Citation Formats


                    Tobin, J. G., Nowak, S., Yu, S-W, Alonso-Mori, R., Kroll, T., Nordlund, D., Weng, T-C, and Sokaras, D. Observation of 5f intermediate coupling in uranium x-ray emission spectroscopy.  United Kingdom: N. p., 2020. 
Web.  doi:10.1088/2399-6528/ab6940.

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                    Tobin, J. G., Nowak, S., Yu, S-W, Alonso-Mori, R., Kroll, T., Nordlund, D., Weng, T-C, & Sokaras, D. Observation of 5f intermediate coupling in uranium x-ray emission spectroscopy.  United Kingdom.  https://doi.org/10.1088/2399-6528/ab6940

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                    Tobin, J. G., Nowak, S., Yu, S-W, Alonso-Mori, R., Kroll, T., Nordlund, D., Weng, T-C, and Sokaras, D. Fri .  
"Observation of 5f intermediate coupling in uranium x-ray emission spectroscopy".  United Kingdom.  https://doi.org/10.1088/2399-6528/ab6940.

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@article{osti_1592176,

  title        = {Observation of 5f intermediate coupling in uranium x-ray emission spectroscopy},

  author       = {Tobin, J. G. and Nowak, S. and Yu, S-W and Alonso-Mori, R. and Kroll, T. and Nordlund, D. and Weng, T-C and Sokaras, D.},

  abstractNote = {The first observation of Intermediate Coupling effects in the occupied 5f states has been made using X-ray Emission Spectroscopy (XES). In the past, the impact of Intermediate Coupling of the 5f states in actinides has long been observed and quantified, using X-ray Absorption Spectroscopy (XAS) to probe the unoccupied 5f states, providing great insight into the enigma of 5f electronic structure, but no measure of its effects in the occupied states had been reported. Moreover, because the 5f occupied states in UF4 are almost completely of 5f5/2 character, the observed effect in XES is twice that in XAS for UF4.},

  doi          = {10.1088/2399-6528/ab6940},

  journal      = {Journal of Physics Communications},

  number       = 1,

  volume       = 4,

  place        = {United Kingdom},

  year         = {Fri Jan 17 00:00:00 EST 2020},

  month        = {Fri Jan 17 00:00:00 EST 2020}

}

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Title: Observation of 5f intermediate coupling in uranium x-ray emission spectroscopy

Abstract

Citation Formats

Electronic structure of solid uranium tetrafluoride UF 4 journal, July 2006

Fluctuating valence in a correlated solid and the anomalous properties of δ-plutonium journal, March 2007

Separate measurement of the 5f5/2 and 5f7/2 unoccupied density of states of UO2 journal, April 2019

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Nature of the Chemical Bond in Uranium Dioxide UO2 journal, May 2005

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The effects of mesoscale confinement in Pu clusters and isolated particles journal, June 2014

Electronic structure of uranium halides and oxyhalides in the solid state. An x-ray photoelectron spectral study of bonding ionicity journal, October 1982

Competition between delocalization and spin-orbit splitting in the actinide 5 f states journal, August 2005

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Confirmation of sample quality: X-ray and ultraviolet photoelectron spectroscopies of uranium dioxide journal, March 2011

Theoretical approaches to x-ray absorption fine structure journal, July 2000

Near-edge x-ray-absorption fine structure in uranium compounds journal, February 1987

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An alternative model for electron correlation in Pu journal, September 2008

Electronic structure of solid uranium tetrafluoride ${UF}_{4}$
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Fluctuating valence in a correlated solid and the anomalous properties of δ-plutonium
journal, March 2007

Separate measurement of the 5f5/2 and 5f7/2 unoccupied density of states of UO2
journal, April 2019

EXAFS investigation of UF4
journal, March 2015

Failure of Russell-Saunders Coupling in the $5 f$ States of Plutonium
journal, May 2003

Angle-resolved photoemission and first-principles electronic structure of single-crystalline $α$ -U(001)
journal, January 2007

Dynamic screening effects in x-ray absorption spectra
journal, March 2003

Relativistic Dirac-Fock expectation values for atoms with Z = 1 to Z = 120
journal, January 1973

The valence-fluctuating ground state of plutonium
journal, July 2015

Nature of the Chemical Bond in Uranium Dioxide UO2
journal, May 2005

The Issue of Pu 5f Occupation
journal, January 2018

Metallic radii and electron configurations of the 5f−6d metals
journal, October 1973

Calculated Bulk Properties of the Actinide Metals
journal, July 1978

Parameter-free calculations of X-ray spectra with FEFF9
journal, January 2010

Multiconfigurational nature of 5f orbitals in uranium and plutonium intermetallics
journal, June 2012

The effects of mesoscale confinement in Pu clusters and isolated particles
journal, June 2014

Electronic structure of uranium halides and oxyhalides in the solid state. An x-ray photoelectron spectral study of bonding ionicity
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Competition between delocalization and spin-orbit splitting in the actinide $5 f$ states
journal, August 2005

Probing actinide electronic structure through pu cluster calculations
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$f$ - $f$ origin of the insulating state in uranium dioxide: X-ray absorption experiments and first-principles calculations
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Theoretical approaches to x-ray absorption fine structure
journal, July 2000

Near-edge x-ray-absorption fine structure in uranium compounds
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