Abstract The interplay between various competing parameters, for example covalency, non-cubic crystal field, and spin-orbit coupling (SOC) leads to fascinating electronic and magnetic phases of matter. In the present work, the effect of these competing parameters on the ground state properties of the systems with d 5 , d 4 , and d 3 electronic configurations are studied using atomic and two-site full multi-orbital man-body electronic Hamiltonian. In order to connect with the real world materials, explicit density functional calculations are employed to study the electronic and the magnetic properties of a series of double perovskite iridates Sr 2 MIrO 6 (M = Ce, Sc, Ca) with formal valences of Ir: Ir 4 + ( d 5 ), Ir 5 + ( d 4 ), and Ir 6 + ( d 3 ). All these iridates facilitate a finite noncubic crystal field and strong Ir-O covalency along with large SOC, thereby offering an excellent platform for the present study. Using the symmetry allowed magnetic structures, the magnetic properties of these materials are studied and compared with the available experimental results. The results of the present work are pertinent to describe the electronic properties of a broad family of spin-orbit coupled materials.

中文翻译：

---

共价键、非立方晶体场和自旋轨道耦合的相互作用：d5、d4 和 d3 双钙钛矿铱酸盐 Sr2MIrO6（M = Ce、Sc、Ca）的比较研究

摘要 各种竞争参数（例如共价性、非立方晶体场和自旋轨道耦合 (SOC)）之间的相互作用导致了物质的迷人电子相和磁相。在目前的工作中，使用原子和双位点全多轨道人体电子哈密顿量研究了这些竞争参数对具有 d 5 、d 4 和 d 3 电子配置的系统基态特性的影响。为了与现实世界的材料联系起来，我们采用显式密度泛函计算来研究一系列具有 Ir 形式化合价的双钙钛矿铱酸盐 Sr 2 MIrO 6 (M = Ce, Sc, Ca) 的电子和磁特性： Ir 4 + (d 5 )、Ir 5 + (d 4 )和Ir 6 + (d 3 )。所有这些铱酸盐促进了有限的非立方晶体场和强的 Ir-O 共价以及大的 SOC，从而为本研究提供了一个极好的平台。使用对称性允许的磁结构，研究这些材料的磁特性并与可用的实验结果进行比较。当前工作的结果与描述一系列自旋轨道耦合材料的电子特性有关。