Spatially Resolved Spectroscopic Characterization of Nanostructured Films by Hyperspectral Dark-Field Microscopy.

Nanostructured films have been widely used for preparing various advanced thin-film devices because of their unique electrical, optical, and plasmonic characteristics associated with the nano-size effect. In situ, nondestructive and high-resolution characterization of nanostructured films is essential for optimizing thin-film device performance. In this work, such thin-film characterization was achieved using a hyperspectral dark-field microscope (HSDFM) that was constructed in our laboratory by integrating a hyperspectral imager with a commercial microscope. The HSDFM allows for high-resolution (Δλ = 0.4 nm) spectral analysis of nanostructured samples in the visible-near-infrared region with a spatial resolution as high as 45 nm × 45 nm (corresponding to a single pixel). Four typical samples were investigated with the HSDFM, including the gold nanoplate array, the self-assembled gold nanoparticle (GNP) sub-monolayer, the sol-gel nanoporous titanium dioxide (TiO2) film, and the layer-stacked molybdenum disulfide (MoS2) sheet. According to the experimental results, the plasmon resonance scattering bands for nanoplate clusters are identical with those for individual gold nanoplates, indicating that the gap between adjacent nanoplates is too large to allow plasmonic coupling between them. A different case was observed with the self-assembled GNP sub-monolayer in which the aggregated clusters with the internal plasmonic interaction show a considerable red-shift of the plasmon resonance band relative to the isolated single GNP. In addition, the protein adsorption on the nanoporous TiO2 film was observed to be inhomogeneous on the microscale, and the stepped boundaries of the MoS2 sheet were clearly observed. A quasi-linear dependence of the single-pixel light intensity on the step height was obtained by combining the HSDFM with atomic force microscopy. The minimum thickness detectable by the present HSDFM is 6.5 nm, corresponding to the 10-layer MoS2 film. The work demonstrated the outstanding applicability of the HSDFM for nanostructured film characterization.