Separate measurement of the 5f5/2 and 5f7/2 unoccupied density of states of UO2

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

doi:10.1016/j.elspec.2019.03.003

Title: Separate measurement of the 5f_5/2 and 5f_7/2 unoccupied density of states of UO₂

Abstract

Coupling High Energy Resolution Fluorescence Detection (HERFD) with electric dipole selection rules, the uranium 5f_5/2 and 5f_7/2 Unoccupied Densities of States (UDOS) have been determined in UF₄, UO₂ and UCd₁₁. Striking changes were observed between UF₄ (5f²) to UCd 11 (5f³), consistent with the Intermediate Coupling Model. Results for UO₂ were confirmed by Bremstrahlung Isochromat Spectroscopy (BIS). This new approach can be a powerful tool for shedding light on the hidden mysteries of Actinides 5f-electrons properties.

Authors:

Tobin, J. G. ^[1]; Nowak, S. ^[2]; Booth, C. H. ^[3]; Bauer, E. D. ^[4]; Yu, S. -W. ^[5]; Alonso-Mori, R. ^[2]; Kroll, T. ^[2]; Nordlund, D. ^[2]; Weng, T. -C. ^[2]; Sokaras, D. ^[2]

Univ. of Wisconsin-Oshkosh, Oshkosh, WI (United States)
SLAC National Accelerator Lab. (SLAC), Menlo Park, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Publication Date:: Sat Mar 16 00:00:00 EDT 2019

Research Org.:: SLAC National Accelerator Lab. (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Org.:: 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 National Nuclear Security Administration (NNSA)

OSTI Identifier:: 1502814

Alternate Identifier(s):: OSTI ID: 1510768; OSTI ID: 1525752; OSTI ID: 1575971

Report Number(s):: LLNL-JRNL-760870
Journal ID: ISSN 0368-2048

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

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Electron Spectroscopy and Related Phenomena

Additional Journal Information:: Journal Volume: 232; Journal Issue: C; Journal ID: ISSN 0368-2048

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 47 OTHER INSTRUMENTATION; X-ray emission; Uranium dioxide; 5f electronic structure; 36 MATERIALS SCIENCE

Citation Formats


                    Tobin, J. G., Nowak, S., Booth, C. H., Bauer, E. D., Yu, S. -W., Alonso-Mori, R., Kroll, T., Nordlund, D., Weng, T. -C., and Sokaras, D. Separate measurement of the 5f5/2 and 5f7/2 unoccupied density of states of UO2.  United States: N. p., 2019. 
Web.  doi:10.1016/j.elspec.2019.03.003.

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                    Tobin, J. G., Nowak, S., Booth, C. H., Bauer, E. D., Yu, S. -W., Alonso-Mori, R., Kroll, T., Nordlund, D., Weng, T. -C., & Sokaras, D. Separate measurement of the 5f5/2 and 5f7/2 unoccupied density of states of UO2.  United States.  https://doi.org/10.1016/j.elspec.2019.03.003

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                    Tobin, J. G., Nowak, S., Booth, C. H., Bauer, E. D., Yu, S. -W., Alonso-Mori, R., Kroll, T., Nordlund, D., Weng, T. -C., and Sokaras, D. Sat .  
"Separate measurement of the 5f5/2 and 5f7/2 unoccupied density of states of UO2".  United States.  https://doi.org/10.1016/j.elspec.2019.03.003.  https://www.osti.gov/servlets/purl/1502814.

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@article{osti_1502814,

  title        = {Separate measurement of the 5f5/2 and 5f7/2 unoccupied density of states of UO2},

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

  abstractNote = {Coupling High Energy Resolution Fluorescence Detection (HERFD) with electric dipole selection rules, the uranium 5f5/2 and 5f7/2 Unoccupied Densities of States (UDOS) have been determined in UF4, UO2 and UCd11. Striking changes were observed between UF4 (5f2) to UCd 11 (5f3), consistent with the Intermediate Coupling Model. Results for UO2 were confirmed by Bremstrahlung Isochromat Spectroscopy (BIS). This new approach can be a powerful tool for shedding light on the hidden mysteries of Actinides 5f-electrons properties.},

  doi          = {10.1016/j.elspec.2019.03.003},

  journal      = {Journal of Electron Spectroscopy and Related Phenomena},

  number       = C,

  volume       = 232,

  place        = {United States},

  year         = {Sat Mar 16 00:00:00 EDT 2019},

  month        = {Sat Mar 16 00:00:00 EDT 2019}

}

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Works referencing / citing this record:

Observation of 5f intermediate coupling in uranium x-ray emission spectroscopy
journal, January 2020

Tobin, J. G.; Nowak, S.; Yu, S-W
Journal of Physics Communications, Vol. 4, Issue 1
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Title: Separate measurement of the 5f5/2 and 5f7/2 unoccupied density of states of UO2

Abstract

Citation Formats

Science-based cleanup of Rocky Flats journal, September 2006

Calculated Bulk Properties of the Actinide Metals journal, July 1978

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

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

Covalency in f-element complexes journal, January 2013

Speciation and Unusual Reactivity in PuO 2+ x journal, June 2003

Absence of magnetic moments in plutonium journal, August 2005

The apparent absence of chemical sensitivity in the 4d and 5d X-ray absorption spectroscopy of uranium compounds journal, June 2014

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

Delocalization and occupancy effects of 5f orbitals in plutonium intermetallics using L3-edge resonant X-ray emission spectroscopy journal, June 2014

Probing 5 f -state configurations in URu 2 Si 2 with U L III -edge resonant x-ray emission spectroscopy journal, July 2016

The role of the 5f valence orbitals of early actinides in chemical bonding journal, July 2017

Chemical State of Complex Uranium Oxides journal, December 2013

Orbital Specificity in the Unoccupied States of UO 2 from Resonant Inverse Photoelectron Spectroscopy journal, October 2011

On the electronic configuration in Pu: spectroscopy and theory journal, February 2008

High-energy spectroscopic study of the occupied and unoccupied 5 f and valence states in Th and U metals journal, March 1980

An instrument for the investigation of actinides with spin resolved photoelectron spectroscopy and bremsstrahlung isochromat spectroscopy journal, September 2011

Resonant x-ray spectroscopy of uranium intermetallics at the M 4 , 5 edges of uranium journal, June 2017

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

Surface degradation of uranium tetrafluoride journal, May 2017

X-ray-absorption sum rules in jj -coupled operators and ground-state moments of actinide ions journal, June 1996

Splittings, Satellites and Fine Structure in the Soft X-ray Spectroscopy of the Actinides journal, June 2013

High pressure effects on U L 3 x-ray absorption in partial fluorescence yield mode and single crystal x-ray diffraction in the heavy fermion compound UCd 11 journal, February 2016

Multi-electronic effects in uranium dioxide from X-ray Emission Spectroscopy journal, April 2013

High resolution 1s core hole X-ray spectroscopy in 3d transition metal complexes—electronic and structural information journal, January 2005

X-ray photoelectron-spectroscopy study of oxides of the transuranium elements Np, Pu, Am, Cm, Bk, and Cf journal, March 1977

5f states with spin-orbit and crystal field splittings journal, May 2019

Observation of 5f intermediate coupling in uranium x-ray emission spectroscopy journal, January 2020

Title: Separate measurement of the 5f_5/2 and 5f_7/2 unoccupied density of states of UO₂

Science-based cleanup of Rocky Flats
journal, September 2006

Calculated Bulk Properties of the Actinide Metals
journal, July 1978

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

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

Covalency in f-element complexes
journal, January 2013

Speciation and Unusual Reactivity in PuO ₂₊ _x
journal, June 2003

Absence of magnetic moments in plutonium
journal, August 2005

The apparent absence of chemical sensitivity in the 4d and 5d X-ray absorption spectroscopy of uranium compounds
journal, June 2014

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

Delocalization and occupancy effects of 5f orbitals in plutonium intermetallics using L3-edge resonant X-ray emission spectroscopy
journal, June 2014

Probing $5 f$ -state configurations in ${URu}_{2} {Si}_{2}$ with U $L_{III}$ -edge resonant x-ray emission spectroscopy
journal, July 2016

The role of the 5f valence orbitals of early actinides in chemical bonding
journal, July 2017

Chemical State of Complex Uranium Oxides
journal, December 2013

Orbital Specificity in the Unoccupied States of ${UO}_{2}$ from Resonant Inverse Photoelectron Spectroscopy
journal, October 2011

On the electronic configuration in Pu: spectroscopy and theory
journal, February 2008

High-energy spectroscopic study of the occupied and unoccupied $5 f$ and valence states in Th and U metals
journal, March 1980

An instrument for the investigation of actinides with spin resolved photoelectron spectroscopy and bremsstrahlung isochromat spectroscopy
journal, September 2011

Resonant x-ray spectroscopy of uranium intermetallics at the $M_{4, 5}$ edges of uranium
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Confirmation of sample quality: X-ray and ultraviolet photoelectron spectroscopies of uranium dioxide
journal, March 2011

Surface degradation of uranium tetrafluoride
journal, May 2017

X-ray-absorption sum rules in $jj$ -coupled operators and ground-state moments of actinide ions
journal, June 1996

Splittings, Satellites and Fine Structure in the Soft X-ray Spectroscopy of the Actinides
journal, June 2013

High pressure effects on U L ₃ x-ray absorption in partial fluorescence yield mode and single crystal x-ray diffraction in the heavy fermion compound UCd ₁₁
journal, February 2016

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journal, April 2013

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journal, January 2005

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journal, March 1977

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journal, January 2020