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Single atoms and few-atom nanoclusters are of high interest in catalysis andplasmonics, but pathways for their fabrication and stable placement remainscarce. We report here the self-assembly of room-temperature-stable singleindium (In) atoms and few-atom In clusters (2-6 atoms) that are anchored tosubstitutional silicon (Si) impurity atoms in suspended monolayer graphenemembranes. Using atomically resolved scanning transmission electron microscopy(STEM), we find that the exact atomic arrangements of the In atoms dependstrongly on the original coordination of the Si anchors in the graphenelattice: Single In atoms and In clusters with 3-fold symmetry readily form on3-fold coordinated Si atoms, whereas 4-fold symmetric clusters are foundattached to 4-fold coordinated Si atoms. All structures are produced by ourfabrication route without the requirement for electron-beam induced materialsmodification. In turn, when activated by electron beam irradiation in the STEM,we observe in situ the formation, restructuring and translation dynamics of theSi-anchored In structures: Hexagon-centered 4-fold symmetric In clusters can(reversibly) transform into In chains or In dimers, whereas C-centered 3-foldsymmetric In clusters can move along the zig-zag direction of the graphenelattice due to the migration of Si atoms during electron-beam irradiation, ortransform to Si-anchored single In atoms. Our results provide a novel frameworkfor the controlled self-assembly and heteroatomic anchoring of single atoms andfew-atom clusters on graphene.

Single indium atoms and few-atom indium clusters anchored onto graphene via silicon heteroatoms