Different mechanisms of A-site and B-site high entropy effect on radiation tolerance of pyrochlores

doi:10.1016/j.jmst.2024.02.002

Abstract

Abstract: The properties of high entropy pyrochlore have been studied extensively, but there is no consistent con-clusion on its radiation tolerance. Besides, the mechanism of the high entropy effect on the radiation tolerance of pyrochlore is still unclear. In this work, combined with experiments and calculations of pyrochlores with similar cationic radius ratios, the A-site and B-site high entropy effects on structural evolution under irradiation are analyzed. In situ irradiation experiments were carried out on A-site high entropy pyrochlores such as (La_0.2 Nd_0.2 Sm_0.2 Gd_0.2Er_0.2)₂ Zr₂ O₇, B-site Gd₂ (Ti_1/3 Sn_1/3 Zr_1/3)₂ O₇, and ternary pyrochlore Sm₂ Zr₂ O₇ and Gd₂ Sn₂ O₇ for comparison. The A-site high entropy pyrochlore can maintain a stable structure under high fluence irradiation like corresponding ternary pyrochlore, demonstrated by high angle annular dark field scanning transmission electron microscopy (HAADF-STEM), energy disper-sive spectroscopy (EDS) mapping and Raman spectrum. The additional irradiation experiments on A-site high entropy pyrochlores (La_1/3 Nd_1/3 Gd_1/3)₂ Zr₂ O₇ and (Nd_1/3 Sm_1/3 Gd_1/3)₂ Zr₂ O₇ also confirm the similarity under irradiation between A-site high entropy and ternary pyrochlores. However, the B-site high entropy pyrochlore Gd2 (Ti_1/3 Sn_1/3 Zr_1/3)₂ O₇ becomes amorphous at exceptionally low irradiation fluences, indicat-ing a significantly distinct radiation tolerance compared with the A-site high entropy. The difference be-tween the A-site and B-site high entropy effect is analyzed from cationic lattice distortion, bond strength, and inner electron binding energy by first-principles calculations. The results reveal the role and mecha-nism of the high entropy effect in pyrochlores and lay a foundation for material design and future appli-cations.

Key words: High entropy pyrochlores, In situ irradiation, Crystal overlap Hamilton population, Electron binding energy

Yuxin Li, Yiming Lei, Hao Xiao, Shuang Zhao, Yugang Wang, Zini Cao, Jie Zhang, Jingyang Wang, Guowei Lu, Liuxuan Cao, Chenxu Wang. Different mechanisms of A-site and B-site high entropy effect on radiation tolerance of pyrochlores[J]. J. Mater. Sci. Technol., 2024, 191: 250-258.

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