From Chemical Complexity to Tunable Magnetic Ordering in Highly Disordered High-Entropy Spinel Oxides
Abstract
High-entropy stabilization chemistry is redefining materials design by transforming configurational disorder, arising from the deliberate incorporation of multiple principal cations, into a thermodynamic advantage that promotes phase stability and enables emergent functionalities. In this work, we investigate the evolution of magnetic ordering in spinel-type high entropy oxides by systematically varying the cation composition of the B site within a fixed high-entropy A-site matrix, (Ni0.2Mg0.2Co0.2Cu0.2Zn0.2)B2O4. Upon introducing multicomponent B-site configurations, we uncover a strikingly linear dependence of the magnetic transition temperature (TC) on the TCs of the corresponding single B-site high-entropy systems. Remarkably, this trend persists even in highly complex (Ni0.2Mg0.2Co0.2Cu0.2Zn0.2)(Cr0.2Mn0.2Fe0.2Ga0.2X0.2)2O4, X = Al and Ti. Despite the material's extremely high degree of disorder, absence of a dominant magnetic ion or a straightforward superexchange pathway, detailed magnetization measurements, low-temperature X-ray magnetic circular dichroism, and neutron powder diffraction studies reveal robust long-range ferrimagnetic ordering. These results reveal an emergent predictability in ferrimagnetic high-entropy spinel oxides, where, despite extreme configurational disorder and competing interactions, robust ferrimagnetic order can arise from, rather than be hindered by, extreme configurational disorder. This establishes a pathway for predictively tuning magnetic transition temperatures in high-entropy oxides beyond conventional ordered systems.
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BibTeX
@misc{sharma2026from,
title = {{From Chemical Complexity to Tunable Magnetic Ordering in Highly Disordered High-Entropy Spinel Oxides}},
author = {Neha Sharma and Sushanta Mandal and Nikita Sharma and Amritpal and Sangeeta Thakur and Viktor Ukleev and Chen Luo and Florin Radu and S. D. Kaushik and Tirthankar Chakraborty and Sanjoy Kr. Mahatha and Denis Pelloquin and Sourav Marik},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.37792},
eprint = {2609.37792},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.37792},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - From Chemical Complexity to Tunable Magnetic Ordering in Highly Disordered High-Entropy Spinel Oxides
AU - Neha Sharma
AU - Sushanta Mandal
AU - Nikita Sharma
AU - Amritpal
AU - Sangeeta Thakur
AU - Viktor Ukleev
AU - Chen Luo
AU - Florin Radu
AU - S. D. Kaushik
AU - Tirthankar Chakraborty
AU - Sanjoy Kr. Mahatha
AU - Denis Pelloquin
AU - Sourav Marik
PY - 2026
DA - 2026/09/29
PB - arXiv
DO - 10.48550/arxiv.2609.37792
UR - https://arxiv.org/abs/2609.37792
AB - High-entropy stabilization chemistry is redefining materials design by transforming configurational disorder, arising from the deliberate incorporation of multiple principal cations, into a thermodynamic advantage that promotes phase stability and enables emergent functionalities. In this work, we investigate the evolution of magnetic ordering in spinel-type high entropy oxides by systematically varying the cation composition of the B site within a fixed high-entropy A-site matrix, (Ni_0.2Mg_0.2Co_0.2Cu_0.2Zn_0.2)B_2O_4. Upon introducing multicomponent B-site configurations, we uncover a strikingly linear dependence of the magnetic transition temperature (T_C) on the T_Cs of the corresponding single B-site high-entropy systems. Remarkably, this trend persists even in highly complex (Ni_0.2Mg_0.2Co_0.2Cu_0.2Zn_0.2)(Cr_0.2Mn_0.2Fe_0.2Ga_0.2X_0.2)_2O_4, X = Al and Ti. Despite the material's extremely high degree of disorder, absence of a dominant magnetic ion or a straightforward superexchange pathway, detailed magnetization measurements, low-temperature X-ray magnetic circular dichroism, and neutron powder diffraction studies reveal robust long-range ferrimagnetic ordering. These results reveal an emergent predictability in ferrimagnetic high-entropy spinel oxides, where, despite extreme configurational disorder and competing interactions, robust ferrimagnetic order can arise from, rather than be hindered by, extreme configurational disorder. This establishes a pathway for predictively tuning magnetic transition temperatures in high-entropy oxides beyond conventional ordered systems.
ER -