skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Pressure Effects on the 4 f Electronic Structure of Light Lanthanides

Abstract

Adopting the satellite structure of the $$\mathcal{Lγ_1}$$ line in nonresonant x-ray emission spectra, we probe the high-pressure evolution of the bare 4f signature of the early light lanthanides at ambient temperature. For Ce and Pr the satellite peak experiences a sudden reduction concurrent with their respective volume collapse (VC) transitions. These new experimental results are supported by calculations using state-of-the-art extended atomic structure codes for Ce and Pr, and also for Nd, which does not exhibit a VC. Here, our work suggests that changes to the 4f occupation are more consistently associated with evolution of the satellite than is the reduction of the 4f moment. Indeed, we show that in the case of Ce, mixing of a higher atomic angular momentum state, driven by the increased hybridization, acts to obscure the expected satellite reduction. These measurements emphasize the importance of a unified study of a full set of microscopic observables to obtain the most discerning test of the underlying, fundamental f-electron phenomena at high pressures.

Authors:
 [1];  [2];  [3];  [1];  [4];  [4];  [5];  [1];  [2];  [1]
  1. Univ. of California, Davis, CA (United States)
  2. Univ. of Washington, Seattle, WA (United States)
  3. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  4. SLAC National Accelerator Lab.(SLAC), Menlo Park, CA (United States)
  5. SLAC National Accelerator Lab.(SLAC), Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab.(SLAC), Menlo Park, CA (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Fusion Energy Sciences (FES) (SC-24)
OSTI Identifier:
1513113
Alternate Identifier(s):
OSTI ID: 1494663; OSTI ID: 1504723
Report Number(s):
LLNL-JRNL-737134
Journal ID: ISSN 0031-9007; PRLTAO
Grant/Contract Number:  
AC52-07NA27344; AC02-06CH11357; AC02-05CH11231; AC02-76SF00515; NA0001974; FG02-99ER45775; SC0002194; SC0016251; DMR-1411336; NA0002908
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 122; Journal Issue: 6; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Chiu, W. -T., Mortensen, D. R., Lipp, M. J., Resta, G., Jia, C. J., Moritz, B., Devereaux, T. P., Savrasov, S. Y., Seidler, G. T., and Scalettar, R. T. Pressure Effects on the 4f Electronic Structure of Light Lanthanides. United States: N. p., 2019. Web. doi:10.1103/physrevlett.122.066401.
Chiu, W. -T., Mortensen, D. R., Lipp, M. J., Resta, G., Jia, C. J., Moritz, B., Devereaux, T. P., Savrasov, S. Y., Seidler, G. T., & Scalettar, R. T. Pressure Effects on the 4f Electronic Structure of Light Lanthanides. United States. doi:10.1103/physrevlett.122.066401.
Chiu, W. -T., Mortensen, D. R., Lipp, M. J., Resta, G., Jia, C. J., Moritz, B., Devereaux, T. P., Savrasov, S. Y., Seidler, G. T., and Scalettar, R. T. Wed . "Pressure Effects on the 4f Electronic Structure of Light Lanthanides". United States. doi:10.1103/physrevlett.122.066401. https://www.osti.gov/servlets/purl/1513113.
@article{osti_1513113,
title = {Pressure Effects on the 4f Electronic Structure of Light Lanthanides},
author = {Chiu, W. -T. and Mortensen, D. R. and Lipp, M. J. and Resta, G. and Jia, C. J. and Moritz, B. and Devereaux, T. P. and Savrasov, S. Y. and Seidler, G. T. and Scalettar, R. T.},
abstractNote = {Adopting the satellite structure of the $\mathcal{Lγ_1}$ line in nonresonant x-ray emission spectra, we probe the high-pressure evolution of the bare 4f signature of the early light lanthanides at ambient temperature. For Ce and Pr the satellite peak experiences a sudden reduction concurrent with their respective volume collapse (VC) transitions. These new experimental results are supported by calculations using state-of-the-art extended atomic structure codes for Ce and Pr, and also for Nd, which does not exhibit a VC. Here, our work suggests that changes to the 4f occupation are more consistently associated with evolution of the satellite than is the reduction of the 4f moment. Indeed, we show that in the case of Ce, mixing of a higher atomic angular momentum state, driven by the increased hybridization, acts to obscure the expected satellite reduction. These measurements emphasize the importance of a unified study of a full set of microscopic observables to obtain the most discerning test of the underlying, fundamental f-electron phenomena at high pressures.},
doi = {10.1103/physrevlett.122.066401},
journal = {Physical Review Letters},
number = 6,
volume = 122,
place = {United States},
year = {2019},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 1 work
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

High pressure phase transformations in neodymium studied in a diamond anvil cell using diamond-coated rhenium gaskets
journal, August 1999

  • Akella, Jagannadham; Weir, Samuel T.; Vohra, Yogesh K.
  • Journal of Physics: Condensed Matter, Vol. 11, Issue 34
  • DOI: 10.1088/0953-8984/11/34/303

Many-body effects in praesodymium core-level spectroscopies of PrO 2
journal, August 1988


The crystal structure and the equation of state of cerium metal in the pressure range 0–46 Gpa
journal, December 1985


Probing the γ α Transition in Bulk Ce under Pressure: A Direct Investigation by Resonant Inelastic X-Ray Scattering
journal, June 2006


Electron spectroscopies for Ce compounds in the impurity model
journal, October 1983


Multiplet effects in X-ray spectroscopy
journal, January 2005


Electrical measurements on praseodymium metal to 179 GPa using designer diamond anvils
journal, February 2004

  • Velisavljevic, Nenad; MacMinn, Kirkland M.; Vohra, Yogesh K.
  • Applied Physics Letters, Vol. 84, Issue 6
  • DOI: 10.1063/1.1645986

Reexamination of the crystal structure of a high‐pressure phase in praseodymium metal
journal, December 1982

  • Smith, Gordon S.; Akella, Jagan
  • Journal of Applied Physics, Vol. 53, Issue 12
  • DOI: 10.1063/1.330393

Rare earth nanoparticles prevent retinal degeneration induced by intracellular peroxides
journal, October 2006

  • Chen, Junping; Patil, Swanand; Seal, Sudipta
  • Nature Nanotechnology, Vol. 1, Issue 2
  • DOI: 10.1038/nnano.2006.91

Superconducting phases of f -electron compounds
journal, November 2009


Lanthanide Complexes in Multifunctional Asymmetric Catalysis
journal, June 2002

  • Shibasaki, Masakatsu; Yoshikawa, Naoki
  • Chemical Reviews, Vol. 102, Issue 6
  • DOI: 10.1021/cr010297z

Resonant inelastic x-ray scattering studies of elementary excitations
journal, June 2011

  • Ament, Luuk J. P.; van Veenendaal, Michel; Devereaux, Thomas P.
  • Reviews of Modern Physics, Vol. 83, Issue 2
  • DOI: 10.1103/RevModPhys.83.705

Concerning the High Pressure Allotropic Modification of Cerium
journal, July 1949


Thermal Signatures of the Kondo Volume Collapse in Cerium
journal, October 2008


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


Theory of the 4d→ 2p X-Ray Emission Spectroscopy in Ce 2 O 3 , Pr 2 O 3 and Dy 2 O 3
journal, June 1995

  • Tanaka, Satoshi; Ogasawara, Haruhiko; Okada, Kozo
  • Journal of the Physical Society of Japan, Vol. 64, Issue 6
  • DOI: 10.1143/JPSJ.64.2225

Nature of the 5 f electrons in the actinide series
journal, April 1975


α-γ transition in Ce. II. A detailed analysis of the Kondo volume-collapse model
journal, September 1992


One-electron physics of the actinides
journal, October 2007


High-pressure crystal structures of actinide elements to 100 GPa
journal, July 2003


Dynamical mean-field theory within the full-potential methods: Electronic structure of CeIrIn 5 , CeCoIn 5 , and CeRhIn 5
journal, May 2010


The α γ Transition in Ce: A Theoretical View from Optical Spectroscopy
journal, January 2005


The Compressibility and Pressure Coefficient of Resistance of Ten Elements
journal, January 1927

  • Bridgman, P. W.
  • Proceedings of the American Academy of Arts and Sciences, Vol. 62, Issue 8
  • DOI: 10.2307/25130122

Recent tests of x-ray spectrometers using polycapillary optics
conference, October 2012

  • Heald, Steve; Seidler, Gerald T.; Mortensen, Devon
  • SPIE Optical Engineering + Applications, SPIE Proceedings
  • DOI: 10.1117/12.929960

Screening of Magnetic Moments in PuAm Alloy: Local Density Approximation and Dynamical Mean Field Theory Study
journal, September 2008


Hidden orbital order in the heavy fermion metal URu2Si2
journal, June 2002

  • Chandra, P.; Coleman, P.; Mydosh, J. A.
  • Nature, Vol. 417, Issue 6891
  • DOI: 10.1038/nature00795

4 f electron delocalization and volume collapse in praseodymium metal
journal, March 2012


and x-ray emission lines of rare-earth trifluorides and
journal, December 1997


Simultaneous electrical and X-ray diffraction studies on neodymium metal to 152 GPa
journal, June 2005

  • Velisavljevic, Nenad; Vohra, Yogesh K.; Weir, Samuel T.
  • High Pressure Research, Vol. 25, Issue 2
  • DOI: 10.1080/08957950500162898

α-uranium phase in compressed neodymium metal
journal, February 2000


Lanthanide amidinates and guanidinates in catalysis and materials science: a continuing success story
journal, January 2012


Structural systematics of 4f and 5f elements under pressure
journal, June 1995


Possible highT c superconductivity in the Ba?La?Cu?O system
journal, June 1986

  • Bednorz, J. G.; M�ller, K. A.
  • Zeitschrift f�r Physik B Condensed Matter, Vol. 64, Issue 2
  • DOI: 10.1007/BF01303701

Phase diagram and equation of state of praseodymium at high pressures and temperatures
journal, April 2003


Spectral and Magnetic Properties of α - and γ -Ce from Dynamical Mean-Field Theory and Local Density Approximation
journal, December 2001


Biological Applications of Rare-Earth Based Nanoparticles
journal, October 2011

  • Bouzigues, Cedric; Gacoin, Thierry; Alexandrou, Antigoni
  • ACS Nano, Vol. 5, Issue 11
  • DOI: 10.1021/nn202378b

Metal-insulator transitions
journal, October 1998

  • Imada, Masatoshi; Fujimori, Atsushi; Tokura, Yoshinori
  • Reviews of Modern Physics, Vol. 70, Issue 4, p. 1039-1263
  • DOI: 10.1103/RevModPhys.70.1039

Localized Magnetic States in Metals
journal, October 1961


Novel reentrant high pressure phase transtion in lanthanum
journal, June 1993


Local-density functional and on-site correlations: The electronic structure of La 2 CuO 4 and LaCuO 3
journal, May 1994


A versatile medium-resolution x-ray emission spectrometer for diamond anvil cell applications
journal, August 2013

  • Mortensen, D. R.; Seidler, G. T.; Bradley, J. A.
  • Review of Scientific Instruments, Vol. 84, Issue 8
  • DOI: 10.1063/1.4819257

Comparison of the high-pressure behavior of the cerium oxides C e 2 O 3 and Ce O 2
journal, February 2016


Ultrapressure equation of state of cerium metal to 208 GPa
journal, February 1999

  • Vohra, Yogesh K.; Beaver, Steven L.; Akella, Jagannadham
  • Journal of Applied Physics, Vol. 85, Issue 4
  • DOI: 10.1063/1.369566

Cerium Volume Collapse: Results from the Merger of Dynamical Mean-Field Theory and Local Density Approximation
journal, December 2001


Relation between the Anderson and Kondo Hamiltonians
journal, September 1966


Rough Compressions of 177 Substances to 40,000 Kg/Cm⁲
journal, January 1948

  • Bridgman, P. W.
  • Proceedings of the American Academy of Arts and Sciences, Vol. 76, Issue 3
  • DOI: 10.2307/20023502

The role of the lanthanides in applied catalysis
journal, December 1986


Volume collapse in the Kondo lattice
journal, July 1982


Comment on “Thermal Signatures of the Kondo Volume Collapse in Cerium”
journal, May 2009


Evidence for 4 f ‐shell delocalization in praseodymium under pressure
journal, July 1981

  • Mao, H. K.; Hazen, R. M.; Bell, P. M.
  • Journal of Applied Physics, Vol. 52, Issue 7
  • DOI: 10.1063/1.329332

Density-functional calculation of the parameters in the Anderson model: Application to Mn in CdTe
journal, January 1989


The α-γ transition in cerium is a Mott transition
journal, September 1974


Kondo Volume Collapse and the γ α Transition in Cerium
journal, October 1982