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We demonstrate rectification ratios ($RR$) of $\gtrsim$1000 at biases of1.3~V in bilayers of \buck deposited on copper. Using scanning tunnelingspectroscopy and first-principles calculations, we show that the strongcoupling between \buck and the Cu(111) surface leads to the metallization ofthe bottom \buck layer, while the molecular orbitals of the top \buck areessentially unaffected. Due to this substrate-induced symmetry breaking and toa tunneling transport mechanism, the system behaves as a hole-blocking layer,with a spatial dependence of the onset voltage on intra-layer coordination.Together with previous observations of strong electron-blocking character ofpentacene/\buck bilayers on Cu(111), this work further demonstrates thepotential of strongly-hybridized, \buck-coated electrodes to harness theelectrical functionality of molecular components.

Spatially-resolved, substrate-induced rectification in C$_{60}$ bilayers on copper