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Mixing two chemical elements at the surface of a substrate is known toproduce rich phase diagrams of surface alloys. Here, we extend the concept ofsurface alloying to the case where the two constituent elements are not bothatoms, but rather one atom (copper) and one molecule (fullerene). Whendeposited at room temperature on a Cu(111) surface, fullerenes intermix withthe metal substrate. Surprisingly, 10 distinct copper-fullerene surface alloysare found to coexist. The structure of these alloys, i.e. their composition andcommensurability relationship with the substrate, is resolved using scanningtunneling microscopy and density functional theory calculations. This diversityin the alloying process is associated to the multiple possibilities a fullerenecan bind to the Cu surface. The molecules are indeed found to have in-plane andout-of-plane positional degree of freedom: the molecular alloys have elasticin-plane properties and can buckle. In addition, the molecules can rotate ontheir binding sites, conferring extra degrees of freedom to the system. Weintroduce a competing-interaction energy model, parametrized against theresults of the \textit{ab initio} calculations, that describes well all thephases we observe experimentally.

journal of physical chemistry. c./journal of physical chemistry. c

Positional and Rotational Molecular Degrees of Freedom in a  Metal-Organic Surface Alloy: the Copper-Fullerene System and its Multiple  Structural Phases