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Lattice-Directed Stabilization of Different Spin-State Phases in Metallo-Supramolecular Chains on Au Surfaces

Jing Liu,* Jie Li, Qiwei Chen, Qiang Xue, Yifan Wang, Bin Di, Yongfeng Wang,* and Kai Wu*


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.