The
production of industrially scalable conductive polymer-based
composites (CPCs), with tailored physicochemical properties, such
as anisotropic conductivity, has proved a formidable challenge in
nanoscience and nanotechnology. This is because the final performance
of such CPCs dramatically depends on the distribution and type of
polymer matrix, the degree of spatial ordering, and the material’s
percolation threshold. By adjusting the concentration of single-walled
carbon nanotubes (SWCNTs) within a hot-drawn poly(vinyl alcohol) (PVA)
composite, we show that a 10-fold increase in the CPC’s conductivity
and a four-fold increase in its anisotropy may be obtained. Using
a combination of Raman spectroscopy, density functional theory (DFT),
and nonequilibrium Green’s function (NEGF)-based methods, we
develop a general ab initio model, which describes qualitatively and
semiquantitatively the measured conductivity of our PVA/SWCNT CPCs.
The success of this model shows that the CPC’s conductivity
is determined by (1) the connectivity of the SWCNT network within
the polymer matrix, (2) the hopping resistance to intertube conductance,
(3) the concentration of SWCNTs in the sample, and (4) the amount
of stretching and concomitant orientational order parameter of the
SWCNTs in the composite. Our combined experimental and theoretical
approach provides a means for designing CPCs with given anisotropic
conductivities based on SWCNTs within different polymer matrices and
should prove highly relevant to a broad academic and industrial community
interested in nanomaterial design.