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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)
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:
1504723
Alternate Identifier(s):
OSTI ID: 1494663
Grant/Contract Number:  
AC52-07NA27344; AC02-06CH11357; AC02-05CH11231; AC02-76SF00515; NA0001974; FG02-99ER45775; SC0002194; SC0016251; DMR-1411336; NA0002908
Resource Type:
Journal Article: 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

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.
@article{osti_1504723,
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},
issn = {0031-9007},
number = 6,
volume = 122,
place = {United States},
year = {2019},
month = {2}
}

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Works referenced in this record:

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