Opposite Polarity Surface Photovoltage of MoS Monolayers on Au Nanodot versus Nanohole Arrays.

We prepared MoS monolayers on Au nanodot (ND) and nanohole (NH) arrays. Both these sample arrays exhibited enhanced photoluminescence intensity compared with that of a bare SiO/Si substrate. The reflectance spectra of MoS/ND and MoS/NH had clear features originating from excitation of localized surface plasmon and propagating surface plasmon polaritons. Notably, the surface photovoltages (SPV) of these hybrid plasmonic nanostructures had opposite polarities, indicating negative and positive charging at MoS/ND and MoS/NH, respectively. Surface potential maps, obtained by Kelvin probe force microscopy, suggested that the potential gradient led to a distinct spatial distribution of photo-generated charges in these two samples under illumination. Furthermore, the local density of photo-generated excitons, as predicted from optical simulations, explained the SPV spectra of MoS/ND and MoS/NH. We show that the geometric configuration of the plasmonic nanostructures modified the polarity of photo-generated excess charges in MoS. These findings point to a useful means of optimizing optoelectronic characteristics and improving the performance of MoS-based plasmonic devices.