rhOver: Determination of magnetic anisotropy and related properties for dysprosium(III) single-ion magnets by semiempirical approaches utilizing Hartree-Fock wave functions,Journal of Computational Chemistry

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rhOver: Determination of magnetic anisotropy and related properties for dysprosium(III) single-ion magnets by semiempirical approaches utilizing Hartree-Fock wave functions
Journal of Computational Chemistry ( IF 3.4 ) Pub Date : 2018-10-23 , DOI: 10.1002/jcc.25565
Michael Böhme ₁ , Winfried Plass ₁

Affiliation

Dysprosium(III) ions are promising candidates for the design of single‐ion magnets (SIMs) as they show an intrinsic strong magnetic anisotropy. However, time‐demanding multireference methods are usually necessary to reproduce low‐lying magnetic states. In this work, we present an improved wave function‐based semiempirical ligand‐field (LF) theory approach to obtain magnetochemical properties of dysprosium(III)‐based SIMs. We reduce the computational effort by replacing the central dysprosium(III) ion with either yttrium(III) or lutetium(III), which allows to obtain a closed‐shell wave function from Hartree–Fock calculations. The wave function is subsequently used to determine a so‐called diamagnetic–electrostatic pseudo‐potential (DEPP) of the compound, which in turn can be applied to LF theory to obtain magnetochemical properties. The presented approach is tested against ab initio CASSCF/RASSI‐SO reference calculations and shows accurate prediction of magnetic anisotropy axes and a significant accuracy improvement as compared to point charge‐based LFT methods. In addition, we also introduce an improved electrostatic (IES) approach, which applies the obtained DEPPs to a known electrostatic method introduced by Chilton et al. (Nat. Commun. 2013, 4, 2551) to obtain the direction of the main anisotropy axis in dysprosium(III)‐based SIMs. © 2018 Wiley Periodicals, Inc.

中文翻译：

rhOver：通过半经验方法利用 Hartree-Fock 波函数确定镝 (III) 单离子磁体的磁各向异性和相关特性

镝 (III) 离子是单离子磁体 (SIM) 设计的有希望的候选者，因为它们显示出固有的强磁各向异性。然而，通常需要耗时的多参考方法来重现低洼地磁状态。在这项工作中，我们提出了一种改进的基于波函数的半经验配体场 (LF) 理论方法来获得基于镝 (III) 的 SIM 的磁化学特性。我们通过用钇 (III) 或镥 (III) 替换中心镝 (III) 离子来减少计算工作量，这允许从 Hartree-Fock 计算中获得闭壳波函数。波函数随后用于确定化合物的所谓抗磁-静电赝势 (DEPP)，进而可以将其应用于 LF 理论以获得磁化学性质。所提出的方法针对 ab initio CASSCF/RASSI-SO 参考计算进行了测试，与基于点电荷的 LFT 方法相比，显示了对磁各向异性轴的准确预测和显着的精度改进。此外，我们还介绍了一种改进的静电 (IES) 方法，该方法将获得的 DEPP 应用于 Chilton 等人介绍的已知静电方法。(Nat. Commun. 2013, 4, 2551) 获得基于镝 (III) 的 SIM 中主要各向异性轴的方向。© 2018 Wiley Periodicals, Inc. 将获得的 DEPP 应用于 Chilton 等人引入的已知静电方法。(Nat. Commun. 2013, 4, 2551) 获得基于镝 (III) 的 SIM 中主要各向异性轴的方向。© 2018 Wiley Periodicals, Inc. 将获得的 DEPP 应用于 Chilton 等人引入的已知静电方法。(Nat. Commun. 2013, 4, 2551) 获得基于镝 (III) 的 SIM 中主要各向异性轴的方向。© 2018 Wiley Periodicals, Inc.

更新日期：2018-10-23

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