Design of high-temperature f-block molecular nanomagnets through the control of vibration-induced spin relaxation
Design of high-temperature f-block molecular nanomagnets through the control of vibration-induced spin relaxation
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DOI：
10.1039/c9sc03133b
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发表时间：
2020-02-14
期刊：
影响因子：
8.4
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
仍然阻碍分子纳米磁体实际应用的主要障碍之一是它们的低温工作温度。在追求合理的策略来设计新的分子纳米磁体与增加阻断温度，从头算方法发挥了重要作用，指导合成工作在实验室阶段。然而，当评估振动引起的自旋弛豫，这些方法仍然是远远不够的计算速度，以提供一个有用的预测框架。在这里，我们提出了一个廉价的第一原理方法，致力于评估振动诱导的自旋弛豫的分子f-块单离子磁体，与只需要一个CASSCF计算的重要优势。该方法说明使用两个案例研究的基础上，铀作为磁性中心。最后，我们提出了在配体环境中的化学修饰，目的是抑制自旋弛豫。
One of the main roadblocks that still hamper the practical use of molecular nanomagnets is their cryogenic working temperature. In the pursuit of rational strategies to design new molecular nanomagnets with increasing blocking temperature, ab initio methodologies play an important role by guiding synthetic efforts at the lab stage. Nevertheless, when evaluating vibration-induced spin relaxation, these methodologies are still far from being computationally fast enough to provide a useful predictive framework. Herein, we present an inexpensive first-principles method devoted to evaluating vibration-induced spin relaxation in molecular f-block single-ion magnets, with the important advantage of requiring only one CASSCF calculation. The method is illustrated using two case studies based on uranium as the magnetic centre. Finally, we propose chemical modifications in the ligand environment with the aim of suppressing spin relaxation.