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arXiv 2004.13050cond-mat.str-el
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4-$d$和5-$d$混合价M $_2$ O $_9$二聚体的软各向异性局部矩

Soft and anisotropic local moments in 4$d$ and 5$d$ mixed-valence M$_2$O$_9$ dimers

Ying Li, Alexander A. Tsirlin, Tusharkanti Dey, Philipp Gegenwart, Roser Valenti, Stephen M. Winter

摘要:

通过有限团簇的精确对角化研究了混合价六方钙钛矿$_3$ $_9$二聚体的电子结构和磁性,其中4PDMATHABMP和5 $d$过渡金属M离子填充不同.我们发现,这种二聚体的磁矩是由一个微妙的相互作用的自旋轨道耦合,洪德耦合,库仑排斥,以及电子填充的M离子。最重要的是,磁矩是各向异性和温度相关的。这种行为是由于自旋轨道耦合,磁场效应,以及存在几个近简并的电子配置,其接近允许占领激发态已经在室温下。该分析与各种基于二聚体的材料的实验磁化率测量是一致的。此外,我们进行了调查的A $_3$ B 'M $_2$ O $_9$材料,并提出基态相图的实验相关的M填充的$d^{4.5}$,$d^{3.5}$和$d^{2.5}$。最后,我们的结果表明,通常应用的居里-外斯定律与恒定的磁矩不能用于这些自旋-轨道耦合材料。

英文摘要:

We investigate via exact diagonalization of finite clusters the electronic structure and magnetism of M$_2$O$_9$ dimers in the mixed-valence hexagonal perovskites A$_3$B'M$_2$O$_9$ for various different fillings of 4$d$ and 5$d$ transition-metal M ions. We find that the magnetic moments of such dimers are determined by a subtle interplay of spin-orbit coupling, Hund's coupling, and Coulomb repulsion, as well as the electron filling of the M ions. Most importantly, the magnetic moments are anisotropic and temperature-dependent. This behavior is a result of spin-orbit coupling, magnetic field effects, and the existence of several nearly-degenerate electronic configurations whose proximity allows occupation of excited states already at room temperature. This analysis is consistent with experimental susceptibility measurements for a variety of dimer-based materials. Furthermore, we perform a survey of A$_3$B'M$_2$O$_9$ materials and propose ground-state phase diagrams for the experimentally relevant M fillings of $d^{4.5}$, $d^{3.5}$ and $d^{2.5}$. Finally, our results show that the usually applied Curie-Weiss law with a constant magnetic moment cannot be used in these spin-orbit-coupled materials.

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