With
the rapid development of materials science, on-demand techniques
are highly needed with the capability to characterize materials in
the micrometer and nanometer scales. In this work, we show that, by
employing a prism geometry, total internal reflection sum frequency
generation (SFG) vibrational spectroscopy allows for characterizing
mesoscopic materials with irregular or complex surfaces. Four representative
examples were presented. First, we reveal that mechanical grinding
can subtly alter the surface molecular structures of original materials.
Second, spin coating can substantially change the surface molecular
structures of particle samples. Third, surface restructuring of carboxylated
multiwalled carbon nanotubes can happen in response to the surrounding
environment. Fourth, surface adsorption and desorption dynamics of
toluene on activated charcoal can be traced. Such experiments demonstrate
that there are still a broad range of research fields ahead SFG can
be directed to, where materials in mesoscopic scales with irregular
or complex surfaces can be studied.