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中心离子上内磁场的各向异性能够对克莱默斯单离子磁体的磁化量子隧穿产生重大影响。

The anisotropy of the internal magnetic field on the central ion is capable of imposing great impact on the quantum tunneling of magnetization of Kramers single-ion magnets.

作者信息

Yin Bing, Luo Lan

机构信息

Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education, College of Chemistry and Materials Science, Northwest University, Xi'an, 710127, P. R. China.

出版信息

Phys Chem Chem Phys. 2021 Feb 4;23(4):3093-3105. doi: 10.1039/d0cp05470d.

DOI:10.1039/d0cp05470d
PMID:33491709
Abstract

In this work, a theoretical method, taking into account the anisotropy of the internal magnetic field (B[combining right harpoon above]int), is proposed to predict the rate of quantum tunneling of magnetization (QTM), i.e., τQTM-1, for Kramers single-ion magnets (SIMs). Direct comparison to both experimental and previous theoretical results of three typical Kramers SIMs indicates the necessity of the inclusion of the anisotropy of B[combining right harpoon above]int for accurate description of QTM. The predictions of the method here are consistent with the theory proposed by Prokof'ev and Stamp (PS). For Kramers SIMs of high magnetic axiality, the QTM rates, predicted by the method here, are almost linearly proportional to the results by the PS method. The dependence of τQTM-1 on various parameters is analyzed for model systems. The averaged magnitude of B[combining right harpoon above]int (Bave) and principal g value of the axial direction (gZ) are the parameters on which τQTM-1 is linearly dependent. The ones on which τQTM-1 is quadratically dependent are gXY, i.e., the principal g value of the transversal direction, and xaniso characterizing the anisotropy of B[combining right harpoon above]int. Compared to Bave and gZ, gXY and xaniso provide a higher order of dependence for QTM. Therefore regulation of the SMM property via introduction of desired values of gXY and xaniso ought to be a strategy more efficient than the one via Bave and gZ. Being different from the one via gXY, the strategy via xaniso to regulate the QTM has been rarely touched upon according to our best knowledge. However, this strategy could also lead to significant improvement since it is the same as gXY in the aspect of the dependence of τQTM-1.

摘要

在这项工作中,提出了一种考虑内部磁场((\vec{B}{int}))各向异性的理论方法,用于预测克莱默斯单离子磁体(SIMs)的磁化量子隧穿速率,即(\tau{QTM}^{-1})。与三种典型克莱默斯SIMs的实验结果和先前的理论结果直接比较表明,为了准确描述量子隧穿,必须考虑(\vec{B}{int})的各向异性。这里该方法的预测结果与普罗科菲耶夫和斯坦普(PS)提出的理论一致。对于高磁轴性的克莱默斯SIMs,这里的方法预测的量子隧穿速率几乎与PS方法的结果呈线性比例关系。分析了模型系统中(\tau{QTM}^{-1})对各种参数的依赖性。(\vec{B}{int})的平均大小((B{ave}))和轴向的主(g)值((g_Z))是(\tau_{QTM}^{-1})线性依赖的参数。(\tau_{QTM}^{-1})二次依赖的参数是横向的主(g)值(g_{XY})以及表征(\vec{B}{int})各向异性的(x{aniso})。与(B_{ave})和(g_Z)相比,(g_{XY})和(x_{aniso})对量子隧穿的依赖性更高。因此,通过引入所需的(g_{XY})和(x_{aniso})值来调节单分子磁体性质应该是一种比通过(B_{ave})和(g_Z)更有效的策略。据我们所知,与通过(g_{XY})的策略不同,通过(x_{aniso})调节量子隧穿的策略很少被提及。然而,由于在(\tau_{QTM}^{-1})的依赖性方面它与(g_{XY})相同,所以该策略也可能导致显著的改进。

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