Bioderived materials have become
an increasingly desirable alternative
to materials sourced from nonrenewable resources. Cellulose nanocrystals
(CNCs), often derived from wood pulp, can be used to manufacture thin
films with applications ranging from optical, protective, and aesthetic
coatings to sensors and batteries. Quantifying the mechanical properties
of CNC films is a necessary step toward improving the quality of these
bioderived films. Because CNCs are highly anisotropic and can subsequently
form highly ordered, aligned structures, an experimental method that
can succinctly determine how film properties change with particle
orientation is of interest. Here, spin coating an aqueous solution
of CNCs onto a silicone elastomer results in a radially aligned particle
assembly. As the local orientation of these aligned, high aspect ratio
particles changes with respect to a uniaxially applied compression,
the mechanical response of the particle assembly was observed to vary
significantly. Applying a lateral compression to a radially aligned
CNC film/elastomer bilayer caused surface buckles to align orthogonal
to the compression direction. The wavelength of these wrinkles, coupled
with the thickness of the film and the modulus of the substrate, is
dictated by the modulus of the film. The modulus as a function of
local CNC alignment and position for each film was thus determined
in a single experiment. These experiments measured a higher modulus
for the film where the orientation of the CNC particles is aligned
parallel to the uniaxial compression direction. Coarse-grained modeling
of closely packed, high aspect ratio particle assemblies supporting
the experimental results agrees with the observed trend. Characterizing
the mechanical properties of CNC films can allow for these green materials
to be further developed for industrial-scale implementation; additionally,
an experimental method is proposed for concisely capturing a range
of modulus values in an anisotropic particle film.