Exploring the High-Temperature Frontier in Molecular Nanomagnets: From Lanthanides to Actinides
Exploring the High-Temperature Frontier in Molecular Nanomagnets: From Lanthanides to Actinides
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DOI：
10.1021/acs.inorgchem.9b01610
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发表时间：
2019-09-16
影响因子：
4.6
通讯作者：
Coronado, Eugenio
中科院分区：
文献类型：
--
作者：
Escalera-Moreno, Luis;Baldovi, Jose J.;Coronado, Eugenio
基于单核金属配合物的分子纳米磁体，也被称为单离子磁体（SIMs），正在跨越分子磁学领域具有挑战性的边界。从实验的角度来看，这类磁性分子已经从类镧配合物扩展到d-过渡金属和类放射线配合物。从理论的角度来看，越来越多的改进模型已经开发出来，我们现在不仅能够计算这些系统的分子结构的基础上的电子结构，而且还揭示了振动在磁弛豫过程中的作用，至少对于镧系和d过渡金属SIMs。这些知识使我们能够优化基于镝的SIMs的行为，直到达到液氮温度以上的磁滞。在这篇文章中，我们简要介绍了该领域理论建模的进展。我们首先回顾了研究这些系统电子结构的开发方法，然后将重点转移到理解和优化振动诱导自旋弛豫的开放问题，特别是在铀基分子纳米磁体中。最后，我们讨论了4f和5f SIMs设计策略的差异，包括对茂金属族的分析。
Molecular nanomagnets based on mononuclear metal complexes, also known as single-ion magnets (SIMs), are crossing challenging boundaries in molecular magnetism. From an experimental point of view, this class of magnetic molecules has expanded from lanthanoid complexes to both d-transition metal and actinoid complexes. From a theoretical point of view, more and more improved models have been developed, and we are now able not only to calculate the electronic structure of these systems on the basis of their molecular structures but also to unveil the role of vibrations in the magnetic relaxation processes, at least for lanthanoid and d-transition metal SIMs. This knowledge has allowed us to optimize the behavior of dysprosocenium-based SIMs until reaching magnetic hysteresis above liquid-nitrogen temperature. In this contribution, we offer a brief perspective of the progress of theoretical modeling in this field. We start by reviewing the developed methodologies to investigate the electronic structures of these systems and then move on focus to the open problem of understanding and optimizing the vibrationally induced spin relaxation, especially in uranium-based molecular nanomagnets. Finally, we discuss the differences in the design strategies for 4f and 5f SIMs, including an analysis of the metallocenium family.