Electron–phonon couplings at C60 interfaces: a case study by two-color, infrared–visible sum–frequency generation spectroscopy

We demonstrate the ability of doubly resonant sum–frequency generation (DR-SFG) to investigate electron–phonon couplings at C 60 –metal interfaces. Due to its coupling to electronic transitions, the totally symmetric A g (2) vibration of C 60 exhibits a huge enhancement of its nonlinear response for sum–frequency energies above the molecular electronic gap. We attribute this resonance to the coupling of the pentagonal pinch mode with the t 1u lowest unoccupied molecular orbital (LUMO) of C 60 .