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Abstract Rare‐earth complexes are vital for separation chemistry and useful in many advanced applications including emission and energy upconversion. Here, 2D rare‐earth clusters having net charges are formed on a metal surface, enabling investigations of their structural and electronic properties on a one‐cluster‐at‐a‐time basis using scanning tunneling microscopy. While these ionic complexes are highly mobile on the surface at ≈100 K, their mobility is greatly reduced at 5 K and reveals stable and self‐limiting clusters. In each cluster, a pair of charged rare‐earth complexes formed by electrostatic and dispersive interactions act as a basic unit, and the clusters are chiral. Unlike other non‐ionic molecular clusters formed on the surfaces, these rare‐earth clusters show mechanical stability. Moreover, their high mobility on the surface suggests that they are in a 2D liquid‐like state.

Rare-earth elements are vital to advanced technological applications ranging from spintronic devices to quantum information science. Here, the authors formed charged rare-earth complexes on a material surface and demonstrated atomically precise control on their rotational dynamics.

Controlling the rotation direction of individual molecular machines requires precise design and manipulation. Here, the authors describe a surface-adsorbed molecular propeller that, upon excitation with a scanning tunneling microscope tip, can rotate clockwise or anticlockwise depending on its chirality, and directly visualize its stepwise rotation with STM images.