The effect of molecular mobility on electronic transport in carbon nanotube-polymer composites and networks

Abstract

A multiscale modeling approach to the prediction of electrical conductivity in carbon nanotube (CNT)–polymer composite materials is developed, which takes into account thermally activated molecular mobility of the matrix and the CNTs. On molecular level, a tight-binding density functional theory and non-equilibrium Green's function method are used to calculate the static electron transmission function in the contact between two metallic carbon nanotubes that corresponds to electron transport at 0 K. For higher temperatures, the statistical distribution of effective contact resistances is considered that originates from thermal fluctuations of intermolecular distances caused by molecular mobility of carbon nanotube and the polymer matrix. Based on this distribution and using effective medium theory, the temperature dependence of macroscopic electrical resistivity for CNT-polymer composites and CNT mats is calculated. The predicted data indicate that the electrical conductivity of the CNT-polymer composites increases linearly with temperature above 50 K, which is in a quantitative agreement with the experiments. Our model predicts a slight nonlinearity in temperature dependence of electric conductivity at low temperatures for percolated composites with small CNT loading. The model also explains the effect of glass transition and other molecular relaxation processes in the polymer matrix on the composite electrical conductivity. The developed multiscale approach integrates the atomistic charge transport mechanisms in percolated CNT-polymer composites with the macroscopic response and thus enables direct comparison of the prediction with the measurements of macroscopic material properties.