Layer-Controlled Intermolecular Coupling and Many-Body Effects in C$_60$ Films

Kavli Affiliate: Alessandra Lanzara
| Summary:
Crystalline C$_60$ is a molecular solid whose electronic properties emerge from the interplay of intermolecular hopping, electron correlations, and electron-vibration coupling. Unlike moir$rmacutee$ van der Waals heterostructures, where interaction strength is commonly tuned by twist angle, molecular materials offer a complementary route in which layer number, molecular orientation, and substrate registry provide experimentally accessible control parameters. Here we present a systematic thickness-dependent angle-resolved photoemission study of C$_60$ films, spanning the monolayer to the bulk limit. The HOMO-derived band exhibits a non-monotonic evolution: the intermediate-thickness film shows larger bandwidth, reduced effective mass, and pronounced gap-like and sub-band features. The experimental trends, together with Holstein-model simulations, point to strengthened effective intermolecular electronic coupling and enhanced electron-phonon-induced spectral renormalization in the intermediate-thickness regime. These results identify a dimensional crossover in C$_60$ films and establish layer number as an effective knob for engineering electronic structure and many-body interactions in molecular thin films.
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