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Hybrid van der Waals (vdW) heterostructures constructed by the integration oforganic molecules and two-dimensional (2D) transition metal dichalcogenide(TMD) materials have useful tunable properties for flexible electronic devices.Due to the chemically inert and atomically smooth nature of the TMD surface,well-defined crystalline organic films form atomically sharp interfacesfacilitating optimal device performance. Here, the surface phase transformationof the supramolecular packing structure of fluorinated fullerene (C60F48) onsingle-layer (SL) tungsten diselenide (WSe2) is revealed by low-temperature(LT) scanning tunnelling microscopy (STM), from thermally stable liquid tosolid phases as the coverage increases. Statistical analysis of theintermolecular interaction potential reveals that the repulsive dipole-dipoleinteraction induced by interfacial charge transfer and substrate-mediatedinteractions play important roles in stabilizing the liquid C60F48 phases.Theoretical calculations further suggest that the dipole moment per C60F48molecule varies with the surface molecule density, and the liquid-solidtransformation could be understood from the perspective of the thermodynamicfree energy for open systems. This study offers new insights into the growthbehaviour at 2D organic/TMD hybrid heterointerfaces.

Liquid-solid surface phase transformation of fluorinated fullerene on monolayer tungsten diselenide