Lattice-Directed Stabilization of Different Spin-State Phases in Metallo-Supramolecular Chains on Au Surfaces
Lattice-Directed Stabilization of Different Spin-State Phases in Metallo-Supramolecular Chains on Au Surfaces
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DOI：
10.1021/acs.chemmater.1c01798
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发表时间：
2021-08
影响因子：
8.6
通讯作者：
Jing Liu;Jie Li;Qiwei Chen;Q. Xue;Y. Wang;Bin Di;Yongfeng Wang;Kai Wu
中科院分区：
文献类型：
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作者：
Jing Liu;Jie Li;Qiwei Chen;Q. Xue;Y. Wang;Bin Di;Yongfeng Wang;Kai Wu
具有特定自旋态有序的分子基纳米结构的可控构建对于自旋电子器件和磁性材料的设计具有重要意义。在这里，我们报告的制造具有不同的自旋态相的Au基板的不同晶格平面上的金属超分子链。在Au（100）和Au（110）上，四羟基苯与Ni配位形成一维分子结构。通过扫描隧道显微镜/光谱和密度泛函理论计算，我们确定了Au（100）和Au（110）上配位链中的Ni原子分别处于低自旋（LS，S= 0）和高自旋（HS，S= 1）态，导致Au（100）上的LS相和Au（110）上的HS相.我们证明了在不同的Au表面上的链中不同的Ni-Ni分离下，不同的自旋态有序在Au衬底上的选择性稳定源于自旋态相的不同基态。这种晶格平面依赖的变化，在镍-镍距离揭示作为结果的链基板的可折叠性。这些研究结果提供了深入了解的关键作用的基板效应在调整表面限制的超分子系统的磁性。
Controlled construction of molecule-based nanostructures with specific spin-state ordering is significant for design of spintronic devices and magnetic materials. Here, we report on the fabrication of metallo-supramolecular chains featuring varied spin-state phases on different lattice planes of the Au substrate. The one-dimensional molecular structures are formed by coordination between deprotonated tetrahydroxybenzene and Ni on Au(100) and Au(110). By employing scanning tunneling microscopy/spectroscopy and density functional theory calculations, we identify Ni atoms in the coordination chains on Au(100) and Au(110) at a low-spin (LS,S= 0) and high-spin (HS,S= 1) state, respectively, giving rise to the LS phase on Au(100) and the HS phase on Au(110). We demonstrate that the selective stabilization of the different spin-state orderings on the Au substrates stems from the distinct ground states of the spin-state phase at varied Ni–Ni separations in the chains on the different Au surfaces. Such a lattice-plane-dependent variation in Ni–Ni distance is revealed as a result of the chain-substrate commensurability. These findings provide insights into the key role of the substrate effect in tuning the magnetic properties of surface-confined supramolecular systems.