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Title: Probing Cerium 4f States across the Volume Collapse Transition by X-ray Raman Scattering

Abstract

Understanding the volume collapse phenomena in rare-earth materials remains an important challenge due to a lack of information on 4f electronic structures at different pressures. Here, we report the first high-pressure inelastic X-ray scattering measurement on elemental cerium (Ce) metal. By overcoming the ultralow signal issue in the X-ray measurement at the Ce N4,5-edge, we observe the changes of unoccupied 4f states across the volume collapse transition around 0.8 GPa. To help resolve the longstanding debate on the Anderson-Kondo and Mott-Hubbard models, we further compare the experiments with extended multiplet calculations that treat both screening channels on equal footing. The results indicate that a modest change in the 4f-5d Kondo coupling can well describe the spectral redistribution across the volume collapse, whereas the hybridization between neighboring atoms in the Hubbard model appears to play a minor role. Our study helps to constrain the theoretical models and opens a promising new route for systematic investigation of volume collapse phenomena in rare-earth materials.

Authors:
 [1];  [2];  [2];  [3];  [1];  [4]; ORCiD logo [4]; ORCiD logo [1];  [1]; ORCiD logo [1];  [1];  [1];  [1];  [5];  [5]; ORCiD logo [2];  [1];  [6]
  1. Center for High-Pressure Science & Technology Advanced Research, Beijing (China)
  2. Univ. of Alabama, Birmingham, AL (United States)
  3. Univ. of North Georgia, Dahlonega, GA (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  5. Inst. of Fluid Physics, Mianyang (China)
  6. Center for High-Pressure Science & Technology Advanced Research, Beijing (China); Carnegie Inst. of Science, Washington, DC (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1671338
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 10; Journal Issue: 24; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; X-rays; Density functional theory; Energy; Chemical calculations; Phase transitions

Citation Formats

Chen, Bijuan, Pärschke, Ekaterina M., Chen, Wei-Chih, Scoggins, Brandon, Li, Bing, Balasubramanian, Mahalingam, Heald, Steve, Zhang, Jianbo, Deng, Hongshan, Sereika, Raimundas, Sorb, Yesudhas, Yin, Xia, Bi, Yan, Jin, Ke, Wu, Qiang, Chen, Cheng-Chien, Ding, Yang, and Mao, Ho-kwang. Probing Cerium 4f States across the Volume Collapse Transition by X-ray Raman Scattering. United States: N. p., 2019. Web. https://doi.org/10.1021/acs.jpclett.9b02819.
Chen, Bijuan, Pärschke, Ekaterina M., Chen, Wei-Chih, Scoggins, Brandon, Li, Bing, Balasubramanian, Mahalingam, Heald, Steve, Zhang, Jianbo, Deng, Hongshan, Sereika, Raimundas, Sorb, Yesudhas, Yin, Xia, Bi, Yan, Jin, Ke, Wu, Qiang, Chen, Cheng-Chien, Ding, Yang, & Mao, Ho-kwang. Probing Cerium 4f States across the Volume Collapse Transition by X-ray Raman Scattering. United States. https://doi.org/10.1021/acs.jpclett.9b02819
Chen, Bijuan, Pärschke, Ekaterina M., Chen, Wei-Chih, Scoggins, Brandon, Li, Bing, Balasubramanian, Mahalingam, Heald, Steve, Zhang, Jianbo, Deng, Hongshan, Sereika, Raimundas, Sorb, Yesudhas, Yin, Xia, Bi, Yan, Jin, Ke, Wu, Qiang, Chen, Cheng-Chien, Ding, Yang, and Mao, Ho-kwang. Mon . "Probing Cerium 4f States across the Volume Collapse Transition by X-ray Raman Scattering". United States. https://doi.org/10.1021/acs.jpclett.9b02819. https://www.osti.gov/servlets/purl/1671338.
@article{osti_1671338,
title = {Probing Cerium 4f States across the Volume Collapse Transition by X-ray Raman Scattering},
author = {Chen, Bijuan and Pärschke, Ekaterina M. and Chen, Wei-Chih and Scoggins, Brandon and Li, Bing and Balasubramanian, Mahalingam and Heald, Steve and Zhang, Jianbo and Deng, Hongshan and Sereika, Raimundas and Sorb, Yesudhas and Yin, Xia and Bi, Yan and Jin, Ke and Wu, Qiang and Chen, Cheng-Chien and Ding, Yang and Mao, Ho-kwang},
abstractNote = {Understanding the volume collapse phenomena in rare-earth materials remains an important challenge due to a lack of information on 4f electronic structures at different pressures. Here, we report the first high-pressure inelastic X-ray scattering measurement on elemental cerium (Ce) metal. By overcoming the ultralow signal issue in the X-ray measurement at the Ce N4,5-edge, we observe the changes of unoccupied 4f states across the volume collapse transition around 0.8 GPa. To help resolve the longstanding debate on the Anderson-Kondo and Mott-Hubbard models, we further compare the experiments with extended multiplet calculations that treat both screening channels on equal footing. The results indicate that a modest change in the 4f-5d Kondo coupling can well describe the spectral redistribution across the volume collapse, whereas the hybridization between neighboring atoms in the Hubbard model appears to play a minor role. Our study helps to constrain the theoretical models and opens a promising new route for systematic investigation of volume collapse phenomena in rare-earth materials.},
doi = {10.1021/acs.jpclett.9b02819},
journal = {Journal of Physical Chemistry Letters},
number = 24,
volume = 10,
place = {United States},
year = {2019},
month = {12}
}

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