Uncovering the Kagome Ferromagnet within a Family of Metal-Organic Frameworks.

Uncovering the Kagome Ferromagnet within a Family of Metal-Organic Frameworks.
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DOI:
10.1021/acs.chemmater.2c00289
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发表时间:
2022-06-28
影响因子:
8.6
通讯作者:
Clark, Lucy
Clark, Lucy
中科院分区:
材料科学2区
文献类型:
--
作者:
Ivko, Samuel A.;Tustain, Katherine;Dolling, Tristan;Abdeldaim, Aly;Mustonen, Otto H. J.;Manuel, Pascal;Wang, Chennan;Luetkens, Hubertus;Clark, Lucy

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铁磁或反铁磁耦合磁矩的Kagome网络代表了追求物质的各种新的量子和拓扑态的重要模型。在这里,我们探索了一族含Cu2+的金属有机骨架(MOF),它们含有由重位有机连接物支撑的Kagome层,通式为Cu3(CO3)2(X)3·2ClO4(MOF-x),其中x是1,2-双(4-吡啶基)乙烷(BPE),1,2-双(4-吡啶基)乙烯(BPY),或4,4‘-偶氮吡啶(Azpy)。尽管进行了十多年的研究,但这些材料中磁交换相互作用的性质仍然不清楚,这意味着潜在的磁性模型是Kagome铁磁还是反铁磁体尚不清楚。利用单晶X射线衍射,我们为这一族材料开发了一种化学上直观的晶体结构。然后,通过磁化率、粉末中子衍射和Muon-Spin谱测量的结合,我们证明了这个家族的磁性基态是由铁磁性Kagome层组成的,这些铁磁性Kagome层通过扩展的有机柱状连接体反铁磁耦合。
Kagome networks of ferromagnetically or antiferromagnetically coupled magnetic moments represent important models in the pursuit of a diverse array of novel quantum and topological states of matter. Here, we explore a family of Cu2+-containing metal–organic frameworks (MOFs) bearing kagome layers pillared by ditopic organic linkers with the general formula Cu3(CO3)2(x)3·2ClO4 (MOF-x), where x is 1,2-bis(4-pyridyl)ethane (bpe), 1,2-bis(4-pyridyl)ethylene (bpy), or 4,4′-azopyridine (azpy). Despite more than a decade of investigation, the nature of the magnetic exchange interactions in these materials remained unclear, meaning that whether the underlying magnetic model is that of an kagome ferromagnet or antiferromagnet is unknown. Using single-crystal X-ray diffraction, we have developed a chemically intuitive crystal structure for this family of materials. Then, through a combination of magnetic susceptibility, powder neutron diffraction, and muon-spin spectroscopy measurements, we show that the magnetic ground state of this family consists of ferromagnetic kagome layers that are coupled antiferromagnetically via their extended organic pillaring linkers.
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