Resonant interaction of molecular vibrations and surface plasmon polaritons: The weak coupling regime

Adjusting the free-electron concentration, the surface plasmon frequency of the semiconductor ZnOGa is tuned into resonance with the molecular vibrations of the n-alkane tetracontane. Closed molecular films deposited on the semiconductor's surface in the monolayer regime generate distinct signatures in total-attenuated-reflection spectra at the frequencies of the symmetric and asymmetric stretching vibrations of the CH2 group. Their line shape undergoes profound changes from absorptive to dispersive and even anti-resonance behavior when moving along the surface- plasmon dispersion by the angel of incidence. We demonstrate that this line shape diversity results from a phase-sensitive perturbation of the surface-plasmon-polariton generation at the molecule/metal interface.