Orientational Growth of Flexible van der Waals Supramolecular Networks

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The capacity for nanopatterning and functionality is a promising facet of supramolecular self‐assembly. However, the formation of molecular frameworks entirely dependent on van der Waals (vdW) interactions is infrequently explored. Herein, 2D vdW supramolecular structures are synthesized through the self‐assembled cocrystallization of C 60 and decanethiol (DT) molecules on Au(111) surface. Notably, the system eliminates the need of functional groups for specific bonding between adjacent units. The conformation C 60 /DT is delicately manipulated by adjusting molecular coverage and annealing temperature. The absence of directional bonding between C 60 and DT molecules facilitates the formation of a variety of stable phases at room temperature (RT), such as 1) porous C 60 networks with thiol‐filled pores and 2) self‐synthesized (C 60 ) n nanochains with thiol spacers interspersed between the chains are achieved and visualized by scanning tunneling microscopic imaging under RT. This innovative integration of the vdW interaction unveils new avenues for developing supramolecular patterns characterized by their comparatively weak but exceptionally adaptable bonding.