David Grégoire, Le Guennic Boris, Reta Daniel
Univ Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes)-UMR 6226, F-35000 Rennes, France.
Faculty of Chemistry, The University of the Basque Country UPV/EHU, Donostia, 20018, Spain.
Chem Commun (Camb). 2024 Oct 15;60(83):11988-11991. doi: 10.1039/d4cc03025g.
Introducing magnetic coupling between lanthanide ions has been shown to yield better-performing single-molecule magnets (SMMs), as exemplified by the CpLnI family of compounds (Cp: pentaisopropylcyclopentadienyl, Ln: Gd, Tb, or Dy). This unique coupling is mediated through an unpaired electron hosted in a σ-like orbital, that results from the two 5d Ln ions, and understanding these interactions holds the key to continue advancing the rational design of SMMs. Here, we focus on the CpGdI spin-only system and apply a recently proposed DFT-based decomposition scheme to assess the chemical and structural factors that affect the magnetic coupling. Based on these, we propose synthetically feasible systems with increased coupling.
已表明引入镧系离子之间的磁耦合可产生性能更好的单分子磁体（SMM），以CpLnI化合物家族（Cp：五异丙基环戊二烯基，Ln：Gd、Tb或Dy）为例。这种独特的耦合是通过一个存在于类似σ轨道中的未成对电子介导的，该轨道由两个5d镧系离子产生，理解这些相互作用是继续推进SMM合理设计的关键。在此，我们聚焦于CpGdI仅自旋体系，并应用最近提出的基于密度泛函理论（DFT）的分解方案来评估影响磁耦合的化学和结构因素。基于这些，我们提出了具有增强耦合的合成可行体系。
