There is growing interest in systems with randomized
responses
for generating physically unclonable functions (PUFs) in anticounterfeiting
and authentication applications. Atomic-level control over its thickness
and unique Raman spectrum make graphene an attractive material for
PUF applications. Herein, we report graphene PUFs that emerge from
two independent stochastic processes. Randomized variations in the
shape and number of graphene adlayers were achieved by exploiting
and improving the mechanistic understanding of the chemical vapor
deposition of graphene. The randomized positioning of the graphene
domains was then facilitated by dewetting the polymer film, followed
by oxygen plasma etching. This approach yielded surfaces with randomly
positioned and shaped graphene islands with varied numbers of layers
and, therefore, Raman spectra. Raman mapping of surfaces resulted
in multicolor images with a high encoding capacity. Advanced feature-matching
algorithms were employed for the authentication of multicolor images.
The use of two independent stochastic processes on a two-dimensional
nanomaterial platform enables the creation of unique and complex surfaces
that excessively challenge clonability.