Strain-Dependent Dielectric Behavior of Carbon Black Reinforced Natural Rubber

The nature of filler-polymer and filler-filler interactions in rubber composites under strain remains an open question in soft matter physics. These interactions are key to explaining the rich variety of complex behavior exhibited by particle-filled rubber products. In this paper we demonstrate a simultaneous dielectric/dynamic mechanical analysis technique (SDMS) which provides new insights into the structure-property relationships of filled rubbers. The complex permittivity of carbon black filled natural rubber has been characterized under a simultaneous tensile strain field (from 0.1% to 50%). The complex permittivity exhibits a dramatic nonlinear dependence on strain coupled with features which are analogous to mechanical strain softening and strain history, namely the "Payne" and "Mullins" effects. The sensitivity of the complex permittivity to such effects is several orders of magnitude greater than in corresponding, traditional mechanical tests. In addition, we demonstrate for the first time that it is possible to use both strain and electrical field frequency as "dipole filters" which can be used to selectively probe the dipoles present at the polymer-filler interface.