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Title: Pressure-induced tuning of lattice distortion in a high-entropy oxide

Abstract

As a new class of multi-principal component oxides with high chemical disorder, high-entropy oxides (HEOs) have attracted much attention. The stability and tunability of their structure and properties are of great interest and importance, but remain unclear. By using in situ synchrotron radiation X-ray diffraction, Raman spectroscopy, ultraviolet–visible absorption spectroscopy, and ex situ high-resolution transmission electron microscopy, here we show the existence of lattice distortion in the crystalline (Ce 0.2La 0.2Pr 0.2Sm 0.2Y 0.2)O 2-δ HEO according to the deviation of bond angles from the ideal values, and discover a pressure-induced continuous tuning of lattice distortion (bond angles) and band gap. As continuous bending of bond angles, pressure eventually induces breakdown of the long-range connectivity of lattice and causes amorphization. The amorphous state can be partially recovered upon decompression, forming glass–nanoceramic composite HEO. These results reveal the unexpected flexibility of the structure and properties of HEOs, which could promote the fundamental understanding and applications of HEOs.

Authors:
; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science - Office of Basic Energy Sciences - Scientific User Facilities Division; National Natural Science Foundation of China (NNSFC); Fundamental Research Funds for the Central Universities; German Research Foundation (DFG); National Science Foundation (NSF); USDOE Office of Science - Office of Basic Energy Sciences - Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1569483
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Communications Chemistry
Additional Journal Information:
Journal Volume: 2; Journal ID: ISSN 2399-3669
Publisher:
Springer Nature
Country of Publication:
United States
Language:
English

Citation Formats

Cheng, Benyuan, Lou, Hongbo, Sarkar, Abhishek, Zeng, Zhidan, Zhang, Fei, Chen, Xiehang, Tang, Lijie, Prakapenka, Vitali, Greenberg, Eran, Wen, Jianguo, Djenadic, Ruzica, Hahn, Horst, and Zeng, Qiaoshi. Pressure-induced tuning of lattice distortion in a high-entropy oxide. United States: N. p., 2019. Web. doi:10.1038/s42004-019-0216-2.
Cheng, Benyuan, Lou, Hongbo, Sarkar, Abhishek, Zeng, Zhidan, Zhang, Fei, Chen, Xiehang, Tang, Lijie, Prakapenka, Vitali, Greenberg, Eran, Wen, Jianguo, Djenadic, Ruzica, Hahn, Horst, & Zeng, Qiaoshi. Pressure-induced tuning of lattice distortion in a high-entropy oxide. United States. doi:10.1038/s42004-019-0216-2.
Cheng, Benyuan, Lou, Hongbo, Sarkar, Abhishek, Zeng, Zhidan, Zhang, Fei, Chen, Xiehang, Tang, Lijie, Prakapenka, Vitali, Greenberg, Eran, Wen, Jianguo, Djenadic, Ruzica, Hahn, Horst, and Zeng, Qiaoshi. Fri . "Pressure-induced tuning of lattice distortion in a high-entropy oxide". United States. doi:10.1038/s42004-019-0216-2.
@article{osti_1569483,
title = {Pressure-induced tuning of lattice distortion in a high-entropy oxide},
author = {Cheng, Benyuan and Lou, Hongbo and Sarkar, Abhishek and Zeng, Zhidan and Zhang, Fei and Chen, Xiehang and Tang, Lijie and Prakapenka, Vitali and Greenberg, Eran and Wen, Jianguo and Djenadic, Ruzica and Hahn, Horst and Zeng, Qiaoshi},
abstractNote = {As a new class of multi-principal component oxides with high chemical disorder, high-entropy oxides (HEOs) have attracted much attention. The stability and tunability of their structure and properties are of great interest and importance, but remain unclear. By using in situ synchrotron radiation X-ray diffraction, Raman spectroscopy, ultraviolet–visible absorption spectroscopy, and ex situ high-resolution transmission electron microscopy, here we show the existence of lattice distortion in the crystalline (Ce0.2La0.2Pr0.2Sm0.2Y0.2)O2-δ HEO according to the deviation of bond angles from the ideal values, and discover a pressure-induced continuous tuning of lattice distortion (bond angles) and band gap. As continuous bending of bond angles, pressure eventually induces breakdown of the long-range connectivity of lattice and causes amorphization. The amorphous state can be partially recovered upon decompression, forming glass–nanoceramic composite HEO. These results reveal the unexpected flexibility of the structure and properties of HEOs, which could promote the fundamental understanding and applications of HEOs.},
doi = {10.1038/s42004-019-0216-2},
journal = {Communications Chemistry},
number = ,
volume = 2,
place = {United States},
year = {2019},
month = {9}
}

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Works referenced in this record:

Nanostructured High-Entropy Alloys with Multiple Principal Elements: Novel Alloy Design Concepts and Outcomes
journal, May 2004

  • Yeh, J.-W.; Chen, S.-K.; Lin, S.-J.
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Pressure-Driven Assembly of Spherical Nanoparticles and Formation of 1D-Nanostructure Arrays
journal, July 2010

  • Wu, Huimeng; Bai, Feng; Sun, Zaicheng
  • Angewandte Chemie International Edition, Vol. 49, Issue 45, p. 8431-8434
  • DOI: 10.1002/anie.201001581