利用第一原理计算和配体场理论对 Cs3CoCl5 中 Co2+ 的光学光谱和自旋-哈密顿参数进行理论研究

IF 3.8 3区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

Optical Materials Pub Date : 2024-11-14 DOI:10.1016/j.optmat.2024.116428

Wang Fang, Heng-Jie Chen, Jia-Wei Zhang

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引用次数: 0

摘要

通过第一原理计算和配体场理论（LFT）相结合的方法，对 Cs3CoCl5 中 Co2+ 基态的全能级、零场分裂（ZFS）参数 D 和自旋共振 g 因子进行了统一计算。在计算中，没有使用可调参数，LFT 计算所需的所有参数都是通过第一性原理计算确定的。通过库仑相互作用、低对称性配体场和自旋轨道耦合（SOC）相互作用产生的构型相互作用都被考虑在内。计算结果与实验观察结果总体吻合。这表明第一原理计算与 LFT 的结合方法不仅能重现实验结果，还能预测多重子分裂的精细能量结构。

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Theoretical studies of optical spectra and spin-Hamiltonian parameters for Co2+ in Cs3CoCl5 with first-principles calculations and ligand field theory

Unified calculations of whole energy levels, zero-field splitting (ZFS) parameter D and spin resonance g factor of the ground state for Co²⁺ in Cs₃CoCl₅ have been carried out by a combined method of the first-principles calculations and ligand field theory (LFT). In the calculations, no adjustable parameter is used and all the parameters needed in the LFT calculation are determined by first-principles calculations. The configuration interaction through Coulomb interaction, low-symmetry ligand field, and spin-orbital coupling (SOC) interaction are taken into account. The calculated results are in good agreement with the experimental observations overall. It demonstrates that the combined method of first-principles calculations with LFT can not only reproduce experimental results but also predict the fine energy structure of multiplet splittings.

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来源期刊

Optical Materials 工程技术-材料科学：综合

CiteScore

6.60

自引率

12.80%

发文量

1265

审稿时长

38 days

期刊介绍： Optical Materials has an open access mirror journal Optical Materials: X, sharing the same aims and scope, editorial team, submission system and rigorous peer review. The purpose of Optical Materials is to provide a means of communication and technology transfer between researchers who are interested in materials for potential device applications. The journal publishes original papers and review articles on the design, synthesis, characterisation and applications of optical materials. OPTICAL MATERIALS focuses on: • Optical Properties of Material Systems; • The Materials Aspects of Optical Phenomena; • The Materials Aspects of Devices and Applications. Authors can submit separate research elements describing their data to Data in Brief and methods to Methods X.