Functionalized
two-dimensional materials (2DMs) are attracting much attention due
to their promising applications in nanoscale devices. Producing continuous
and homogeneous surface assemblies with a high degree of order has
been challenging. In this work, we demonstrate that by noncovalently
self-assembling molecular platforms on 2DMs, high-quality and highly
ordered monolayers can be generated. The high degree of order and
uniformity of the self-assembled monolayer layers were confirmed by
a variety of analytic techniques including time-of-flight secondary
ion mass spectrometry, scanning tunnelling microscopy, X-ray photoelectron
spectroscopy, and atomic force microscopy. Furthermore, by selectively
enhancing the molecular vibrations of the molecular platform, via
a combination of graphene-enhanced Raman spectroscopy (GERS) and surface-enhanced
Raman spectroscopy (SERS), we were able to determine the orientation
of self-assembled molecular platforms with respect to the surface
normal. The selective enhancement of the vibrational modes occurs
by taking advantage of the distance dependence of the Raman enhancement
either by the graphene surface (GERS) or the silver nanoparticules
(SERS) that are located on top of the self-assembled monolayer.