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Local structural distortions drive magnetic molecular field in compositionally complex spinel oxide

Materials Science 2025-04-11 v3 Strongly Correlated Electrons

Abstract

Understanding how local distortions determine the functional properties of high entropy materials, containing five or more elements at a crystallographic site, is an open challenge. We address this for a compositionally complex spinel oxide (Mn0.2_{0.2}Co0.2_{0.2}Ni0.2_{0.2}Cu0.2_{0.2}Zn0.2_{0.2})Cr2_2O4_4 (A5A^5Cr2_2O4_4). By comparatively examining extended X-ray absorption fine structure on A5A^5Cr2_2O4_4 and its parent counterparts AACr2_2O4_4 along with density functional theory calculations for multiple configurations, we find that the element-specific distortions go beyond the first neighbor. Specifically, the strong Jahn-Teller distortion present in CuCr2_2O4_4 is found to be completely suppressed in A5A^5Cr2_2O4_4. Instead, there is a broad distribution of Cu-O and Cu-Cr bond distances while other AA-O distances acquire certain specific values. This study demonstrates the additional flexibility of a cationic sublattice in maintaining a uniform long-range structure, in contrast to previous reports showing only the accommodative anionic sublattice. Remarkably, despite the presence of multiple magnetic ions and variable bond lengths, the mean field magnetic interactions of A5A^5Cr2_2O4_4 exhibit a striking resemblance to those of NiCr2_2O4_4. This compelling observation originates from the comparability of bond lengths around Cr in both materials. Our study paves the way for a deeper understanding of the impact of local structural distortions in compositionally complex quantum materials, enabling the targeted design with tailored properties.

Keywords

Cite

@article{arxiv.2406.01156,
  title  = {Local structural distortions drive magnetic molecular field in compositionally complex spinel oxide},
  author = {Rukma Nevgi and Subha Dey and Nandana Bhattacharya and Soheil Ershadrad and Tinku Dan and Sujay Chakravarty and S. D. Kaushik and Christoph Klewe and George E. Sterbinsky and Biplab Sanyal and Srimanta Middey},
  journal= {arXiv preprint arXiv:2406.01156},
  year   = {2025}
}
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