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首页> 外文期刊>Chemistry: A European journal >Switching of Single-Molecule Magnetic Properties of Tb~(III)- Porphyrin Double-Decker Complexes and Observation of Their Supramolecular Structures on a Carbon Surface
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Switching of Single-Molecule Magnetic Properties of Tb~(III)- Porphyrin Double-Decker Complexes and Observation of Their Supramolecular Structures on a Carbon Surface

机译：Tb〜（III）-卟啉双层配合物单分子磁性的转换及其在碳表面上超分子结构的观察

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Double-decker complexes based on single-molecule magnets (SMMs) are a class of highly promising molecules for applications in molecular spintronics, wherein control of both the ligand oxidative states and the 2D supramolecular structure on carbon materials is of great importance. This study focuses on the synthesis and study of 2,3,7,8,12,13,17,18-octaethylporphyrin (OEP)-Tb~(III) doubledecker complexes with different electronic structures comprising protonated, anionic, and radical forms. Magnetic susceptibility measurements revealed that only the anionic and radical forms of the OEP-Tb~(III) double-decker complexes exhibited SMM properties. The barrier heights for magnetic moment reversal were estimated to be 207 and 215 cm~(-1) for the anionic and radical forms, respectively. Scanning tunneling microscopy (STM) investigations revealed that these OEP-Tb~(III) complexes form well-ordered monolayers upon simple dropcasting from dilute dichloromethane solutions. All three complexes form an isomorphic pseudo-hexagonal 2D pattern, regardless of the differences in the electronic structures of their porphyrin-Tb cores. This finding is of interest for SMM technology as ultrathin films of these materials undergoing chemical transformations will not require any detrimental reorganization. Finally, we demonstrate self-assembly of the protonated 5,15-bisdodecylporphyrin (BDP)- Tb~(III) double-decker complex as an example of successful supramolecular design to achieve controlled alignment of SMM-active sites.
机译：基于单分子磁体（SMM）的双层配合物是一类非常有前途的分子，可用于分子自旋电子学，其中碳材料上的配体氧化态和2D超分子结构的控制非常重要。这项研究致力于合成和研究具有不同电子结构的2,3,7,8,12,13,17,18-八乙基卟啉（OEP）-Tb〜（III）双层配合物，包括质子化，阴离子和自由基形式。磁化率测量表明，只有OEP-Tb〜（III）双层配合物的阴离子和自由基形式表现出SMM性质。阴离子和自由基形式的磁矩反转的势垒高度估计分别为207和215 cm〜（-1）。扫描隧道显微镜（STM）研究表明，这些OEP-Tb〜（III）络合物在从稀二氯甲烷溶液中进行简单滴铸后就形成了有序的单分子层。不论它们的卟啉-Tb核的电子结构如何不同，这三个复合物均形成同构的伪六边形二维图形。该发现对于SMM技术很有意义，因为这些材料的超薄膜经过化学转化将不需要任何有害的重组。最后，我们证明了质子化的5,15-双十二烷基卟啉（BDP）-Tb〜（III）双层复合物的自组装，作为成功实现超分子设计以实现SMM活性位点受控对齐的一个例子。

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