Pressure Effects on the 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:
-
- Univ. of California, Davis, CA (United States)
- Univ. of Washington, Seattle, WA (United States)
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES); Stanford Univ., CA (United States). Geballe Lab. for Advanced Materials; Stanford Univ., CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Univ. of California, Davis, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Fusion Energy Sciences (FES)
- OSTI Identifier:
- 1513113
- Alternate Identifier(s):
- OSTI ID: 1494663; OSTI ID: 1504723; OSTI ID: 1755099
- Report Number(s):
- LLNL-JRNL-737134
Journal ID: ISSN 0031-9007; PRLTAO; 890158
- 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. https://doi.org/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. https://doi.org/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 = {Wed Feb 13 00:00:00 EST 2019},
month = {Wed Feb 13 00:00:00 EST 2019}
}
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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
Many-body effects in praesodymium core-level spectroscopies of
journal, August 1988
- Bianconi, A.; Kotani, A.; Okada, K.
- Physical Review B, Vol. 38, Issue 5
The crystal structure and the equation of state of cerium metal in the pressure range 0–46 Gpa
journal, December 1985
- Olsen, J. Staun; Gerward, L.; Benedict, U.
- Physica B+C, Vol. 133, Issue 2-3
Probing the Transition in Bulk Ce under Pressure: A Direct Investigation by Resonant Inelastic X-Ray Scattering
journal, June 2006
- Rueff, J. -P.; Itié, J. -P.; Taguchi, M.
- Physical Review Letters, Vol. 96, Issue 23
Electron spectroscopies for Ce compounds in the impurity model
journal, October 1983
- Gunnarsson, O.; Schönhammer, K.
- Physical Review B, Vol. 28, Issue 8
Multiplet effects in X-ray spectroscopy
journal, January 2005
- Groot, Frank de
- Coordination Chemistry Reviews, Vol. 249, Issue 1-2
Competition between Kondo and RKKY exchange couplings in alloys: Density functional theory with static Hartree-Fock and dynamic Hubbard-I approximations
journal, August 2008
- Han, Myung Joon; Wan, Xiangang; Savrasov, Sergej Y.
- Physical Review B, Vol. 78, Issue 6
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
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
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
Superconducting phases of -electron compounds
journal, November 2009
- Pfleiderer, Christian
- Reviews of Modern Physics, Vol. 81, Issue 4
Lanthanide Complexes in Multifunctional Asymmetric Catalysis
journal, June 2002
- Shibasaki, Masakatsu; Yoshikawa, Naoki
- Chemical Reviews, Vol. 102, Issue 6
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
Concerning the High Pressure Allotropic Modification of Cerium
journal, July 1949
- Lawson, A. W.; Tang, Ting-Yuan
- Physical Review, Vol. 76, Issue 2
Thermal Signatures of the Kondo Volume Collapse in Cerium
journal, October 2008
- Lipp, M. J.; Jackson, D.; Cynn, H.
- Physical Review Letters, Vol. 101, Issue 16
High resolution 1s core hole X-ray spectroscopy in 3d transition metal complexes—electronic and structural information
journal, January 2005
- Glatzel, Pieter; Bergmann, Uwe
- Coordination Chemistry Reviews, Vol. 249, Issue 1-2
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
Nature of the electrons in the actinide series
journal, April 1975
- Johansson, Börje
- Physical Review B, Vol. 11, Issue 8
α-γ transition in Ce. II. A detailed analysis of the Kondo volume-collapse model
journal, September 1992
- Allen, J. W.; Liu, L. Z.
- Physical Review B, Vol. 46, Issue 9
One-electron physics of the actinides
journal, October 2007
- Toropova, A.; Marianetti, C. A.; Haule, K.
- Physical Review B, Vol. 76, Issue 15
High-pressure crystal structures of actinide elements to 100 GPa
journal, July 2003
- Lindbaum, A.; Heathman, S.; Bihan, T. Le
- Journal of Physics: Condensed Matter, Vol. 15, Issue 28
Dynamical mean-field theory within the full-potential methods: Electronic structure of , , and
journal, May 2010
- Haule, Kristjan; Yee, Chuck-Hou; Kim, Kyoo
- Physical Review B, Vol. 81, Issue 19
The Transition in Ce: A Theoretical View from Optical Spectroscopy
journal, January 2005
- Haule, Kristjan; Oudovenko, Viktor; Savrasov, Sergej Y.
- Physical Review Letters, Vol. 94, Issue 3
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
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
Thermodynamic and spectral properties of compressed Ce calculated using a combined local-density approximation and dynamical mean-field theory
journal, February 2003
- McMahan, A. K.; Held, K.; Scalettar, R. T.
- Physical Review B, Vol. 67, Issue 7
Screening of Magnetic Moments in PuAm Alloy: Local Density Approximation and Dynamical Mean Field Theory Study
journal, September 2008
- Shim, J. H.; Haule, K.; Savrasov, S.
- Physical Review Letters, Vol. 101, Issue 12
Hidden orbital order in the heavy fermion metal URu2Si2
journal, June 2002
- Chandra, P.; Coleman, P.; Mydosh, J. A.
- Nature, Vol. 417, Issue 6891
New high-temperature superconductors based on rare-earth and transition metal oxyarsenides and related phases: synthesis, properties and simulations
journal, December 2008
- Ivanovskii, Alexander L.
- Physics-Uspekhi, Vol. 51, Issue 12
electron delocalization and volume collapse in praseodymium metal
journal, March 2012
- Bradley, Joseph A.; Moore, Kevin T.; Lipp, Magnus J.
- Physical Review B, Vol. 85, Issue 10
and x-ray emission lines of rare-earth trifluorides and
journal, December 1997
- Jouda, K.; Tanaka, S.; Aita, O.
- Journal of Physics: Condensed Matter, Vol. 9, Issue 48
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
α-uranium phase in compressed neodymium metal
journal, February 2000
- Chesnut, Gary N.; Vohra, Yogesh K.
- Physical Review B, Vol. 61, Issue 6
Lanthanide amidinates and guanidinates in catalysis and materials science: a continuing success story
journal, January 2012
- Edelmann, Frank T.
- Chemical Society Reviews, Vol. 41, Issue 23
Structural systematics of 4f and 5f elements under pressure
journal, June 1995
- Holzapfel, W. B.
- Journal of Alloys and Compounds, Vol. 223, Issue 2
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
Phase diagram and equation of state of praseodymium at high pressures and temperatures
journal, April 2003
- Baer, Bruce J.; Cynn, Hyunchae; Iota, Valentin
- Physical Review B, Vol. 67, Issue 13
Spectral and Magnetic Properties of - and -Ce from Dynamical Mean-Field Theory and Local Density Approximation
journal, December 2001
- Zölfl, M. B.; Nekrasov, I. A.; Pruschke, Th.
- Physical Review Letters, Vol. 87, Issue 27
Biological Applications of Rare-Earth Based Nanoparticles
journal, October 2011
- Bouzigues, Cedric; Gacoin, Thierry; Alexandrou, Antigoni
- ACS Nano, Vol. 5, Issue 11
Metal-insulator transitions
journal, October 1998
- Imada, Masatoshi; Fujimori, Atsushi; Tokura, Yoshinori
- Reviews of Modern Physics, Vol. 70, Issue 4, p. 1039-1263
Localized Magnetic States in Metals
journal, October 1961
- Anderson, P. W.
- Physical Review, Vol. 124, Issue 1
Novel reentrant high pressure phase transtion in lanthanum
journal, June 1993
- Porsch, F.; Holzapfel, W. B.
- Physical Review Letters, Vol. 70, Issue 26
Local-density functional and on-site correlations: The electronic structure of and
journal, May 1994
- Czyżyk, M. T.; Sawatzky, G. A.
- Physical Review B, Vol. 49, Issue 20
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
Comparison of the high-pressure behavior of the cerium oxides and
journal, February 2016
- Lipp, M. J.; Jeffries, J. R.; Cynn, H.
- Physical Review B, Vol. 93, Issue 6
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
Cerium Volume Collapse: Results from the Merger of Dynamical Mean-Field Theory and Local Density Approximation
journal, December 2001
- Held, K.; McMahan, A. K.; Scalettar, R. T.
- Physical Review Letters, Vol. 87, Issue 27
Relation between the Anderson and Kondo Hamiltonians
journal, September 1966
- Schrieffer, J. R.; Wolff, P. A.
- Physical Review, Vol. 149, Issue 2
Combined local-density and dynamical mean field theory calculations for the compressed lanthanides Ce, Pr, and Nd
journal, September 2005
- McMahan, A. K.
- Physical Review B, Vol. 72, Issue 11
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
The role of the lanthanides in applied catalysis
journal, December 1986
- Kilbourn, Barry T.
- Journal of the Less Common Metals, Vol. 126
Volume collapse in the Kondo lattice
journal, July 1982
- Lavagna, M.; Lacroix, C.; Cyrot, M.
- Physics Letters A, Vol. 90, Issue 4
Comment on “Thermal Signatures of the Kondo Volume Collapse in Cerium”
journal, May 2009
- Johansson, B.; Ruban, A. V.; Abrikosov, I. A.
- Physical Review Letters, Vol. 102, Issue 18
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
Density-functional calculation of the parameters in the Anderson model: Application to Mn in CdTe
journal, January 1989
- Gunnarsson, O.; Andersen, O. K.; Jepsen, O.
- Physical Review B, Vol. 39, Issue 3
The α-γ transition in cerium is a Mott transition
journal, September 1974
- Johansson, Börje
- Philosophical Magazine, Vol. 30, Issue 3
Kondo Volume Collapse and the Transition in Cerium
journal, October 1982
- Allen, J. W.; Martin, Richard M.
- Physical Review Letters, Vol. 49, Issue 15
The Theory of Atomic Structure and Spectra
book, December 1981
- Cowan, Robert D.
- Los Alamos Series in Basic and Applied Sciences, Vol. 3
Metal-insulator transitions
journal, June 1991
- Paesler, Michael
- Journal of Non-Crystalline Solids, Vol. 130, Issue 1
Cerium Volume Collapse: Results from the Merger of Dynamical Mean-Field Theory and Local Density Approximation
text, January 2001
- Held, K.; McMahan, A. K.; Scalettar, R. T.
- The American Physical Society
New high-temperature superconductors based on rare earth and transition metal oxyarsenides and related phases: synthesis, properties and simulation [Novye vysokotemperaturnye sverkhprovodniki na osnove oksiarsenidov redkozemel'nykh i perekhodnykh metallov i rodstvennykh faz: sintez, svoistva i modelirovanie]
journal, January 2008
- Ivanovskii, A. L.
- Uspekhi Fizicheskih Nauk, Vol. 178, Issue 12
One-Electron Physics of the Actinides
text, January 2007
- Toropova, A.; Marianetti, C. A.; Haule, K.
- arXiv