While the green production
and application of 2D functional nanomaterials,
such as graphene flakes, in films for stretchable and wearable technologies
is a promising platform for advanced technologies, there are still
challenges involved in the processing of the deposited material to
improve properties such as electrical conductivity. In applications
such as wearable biomedical and flexible energy devices, the widely
used flexible and stretchable substrate materials are incompatible
with high-temperature processing traditionally employed to improve
the electrical properties, which necessitates alternative manufacturing
approaches and new steps for enhancing the film functionality. We
hypothesize that a mechanical stimulus, in the form of substrate straining,
may provide such a low-energy approach for modifying deposited film
properties through increased flake packing and reorientation. To this
end, graphene flakes were exfoliated using an unexplored combination
of ethanol and cellulose acetate butyrate for morphological and percolative
electrical characterization prior to application on polydimethylsiloxane
(PDMS) substrates as a flexible and stretchable electrically conductive
platform. The deposited percolative free-standing films on PDMS were
characterized via in situ resistance strain monitoring and surface
morphology measurements over numerous strain cycles, with parameters
extracted describing the dynamic modulation of the film’s electrical
properties. A reduction in the film resistance and strain gauge factor
was found to correlate with the surface roughness and densification
of a sample’s (sub)surface and the applied strain. High surface
roughness samples exhibited enhanced reduction in resistance as well
as increased sensitivity to strain compared to samples with low surface
roughness, corresponding to surface smoothing, which is related to
the dynamic settling of graphene flakes on the substrate surface.
This procedure of incorporating strain as a mechanical stimulus may
find application as a manufacturing tool/step for the routine fabrication
of stretchable and wearable devices, as a low energy and compatible
approach, for enhancing the properties of such devices for either
high sensitivity or low sensitivity of electrical resistance to substrate
strain.