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Collective molecular physical properties can be enhanced from their intrinsic characteristics by templating at material interfaces. Here we report how a black phosphorous (BP) substrate concatenates a nearly-free-electron (NFE) like conduction band of a C 60  monolayer. Scanning tunneling microscopy reveals the C 60  lowest unoccupied molecular orbital (LUMO) band is strongly delocalized in two-dimensions, which is unprecedented for a molecular semiconductor. Experiment and theory show van der Waals forces between C 60  and BP reduce the inter-C 60  distance and cause mutual orientation, thereby optimizing the π-π wave function overlap and forming the NFE-like band. Electronic structure and carrier mobility calculations predict that the NFE band of C 60  acquires an effective mass of 0.53–0.70  m  e  ( m  e  is the mass of free electrons), and has carrier mobility of ~200 to 440 cm 2 V −1 s −1 . The substrate-mediated intermolecular van der Waals interactions provide a route to enhance charge delocalization in fullerenes and other organic semiconductors.

Realizing nearly-free-electron like conduction band in a molecular film through mediating intermolecular van der Waals interactions