Visualization of surface plasmon polariton (SPP) propagation at dielectric/metal interfaces is indispensable in providing opportunities for the precise designing and controlling of the functionalities of future plasmonic nanodevices. Here, we report the visualization of SPPs propagating along the buried organic/metal interface of fullerene (C60)/Au(111), through dual-colored two-photon photoemission electron microscopy (2P-PEEM) which precisely visualizes the SPP propagation of plasmonic metal nanostructures. Although SPPs excited by near-infrared photons at the few monolayer C60/Au(111) interface are clearly visualized as interference beat patterns between the SPPs and incident light, faithfully reflecting SPP properties modulated by the overlayer, photoemission signals are suppressed for thicker C60 films, due to less valence electrons participating in 2P-photoemission processes. With the use of silver (Agn (n = 21 and 55)) nanoclusters, which exhibit enhancement of overall photoemission intensities due to localized surface plasmons functioning as SPP sensitizers, it is revealed that the 2P-PEEM is applicable to the imaging of SPPs for thick C60/Au(111) interfaces, where SPP properties are hardly modulated by the added small amount (∼0.1 monolayer) of Agn sensitizers.
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