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从化学复杂性到高度无序高熵尖晶石氧化物中的可调磁有序

From Chemical Complexity to Tunable Magnetic Ordering in Highly Disordered High-Entropy Spinel Oxides

Neha Sharma, Sushanta Mandal, Nikita Sharma, Amritpal, Sangeeta Thakur, Viktor Ukleev, Chen Luo, Florin Radu, S. D. Kaushik, Tirthankar Chakraborty, Sanjoy Kr. Mahatha, Denis Pelloquin, Sourav Marik

arXiv 2609.37792首次发表:更新:

发表机构

Thapar Institute of Engineering and Technology; UGC-DAE Consortium for Scientific Research; Freie Universität Berlin; Helmholtz Zentrum Berlin für Materialien und Energie; Normandie University(塔帕尔工程技术学院; UGC-DAE科学研究联盟; 柏林自由大学; 柏林亥姆霍兹材料与能源中心; 诺曼底大学)

机构由 AI 辅助整理,请以论文原文为准。

AI 中文总结

本研究通过系统改变高熵尖晶石氧化物B位组成,发现磁转变温度与单B位体系呈线性关系,即使在极端无序下仍保持稳健亚铁磁有序,为可预测调控磁转变温度开辟了新途径。

AI 中文摘要

高熵稳定化学通过将多种主阳离子的有意引入所产生的构型无序转化为促进相稳定性并实现新兴功能的热力学优势,正在重新定义材料设计。在本工作中,我们通过在固定的高熵A位矩阵(Ni$_{0.2}$Mg$_{0.2}$Co$_{0.2}$Cu$_{0.2}$Zn$_{0.2}$)B$_2$O$_4$内系统改变B位阳离子组成,研究了尖晶石型高熵氧化物中磁有序的演化。引入多组分B位构型后,我们发现磁转变温度(T$_C$)与相应单B位高熵体系的T$_C$s之间存在显著的线性依赖关系。值得注意的是,即使在高度复杂的(Ni$_{0.2}$Mg$_{0.2}$Co$_{0.2}$Cu$_{0.2}$Zn$_{0.2}$)(Cr$_{0.2}$Mn$_{0.2}$Fe$_{0.2}$Ga$_{0.2}$X$_{0.2}$)$_2$O$_4$(X = Al和Ti)中,这一趋势依然存在。尽管该材料具有极高的无序度、缺乏主导磁性离子或直接的超交换路径,详细的磁化测量、低温X射线磁圆二色性和中子粉末衍射研究揭示了稳健的长程亚铁磁有序。这些结果揭示了亚铁磁高熵尖晶石氧化物中一种新兴的可预测性,即在极端构型无序和竞争相互作用下,稳健的亚铁磁有序可以源于而非受阻碍于极端构型无序。这为在高熵氧化物中超越传统有序体系预测性调控磁转变温度建立了途径。

英文摘要

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$_{0.2}$Mg$_{0.2}$Co$_{0.2}$Cu$_{0.2}$Zn$_{0.2}$)B$_2$O$_4$. Upon introducing multicomponent B-site configurations, we uncover a strikingly linear dependence of the magnetic transition temperature (T$_C$) on the T$_C$s of the corresponding single B-site high-entropy systems. Remarkably, this trend persists even in highly complex (Ni$_{0.2}$Mg$_{0.2}$Co$_{0.2}$Cu$_{0.2}$Zn$_{0.2}$)(Cr$_{0.2}$Mn$_{0.2}$Fe$_{0.2}$Ga$_{0.2}$X$_{0.2}$)$_2$O$_4$, 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.

论文原文

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