Variable-temperature measurements of the dielectric relaxation in carbon black loaded epoxy composites

Technologically, an understanding of the temperature influence on the transport properties is essential to the study of many random conductor-insulator composites, while fundamentally it is related to a variety of questions in statistical physics, dielectrics, and materials science, to name a few. Variable-temperature measurements of the frequency dependent complex effective permittivity were performed on amine-cured epoxy resins loaded with carbon black (CB). Two series of prepercolative samples differing from the kind of CB particles (Raven 2000 and Raven 5000) mixed in an amine-cured epoxy matrix (diglycidylic ether of bisphenol F) were studied. In this effort to contribute to our understanding of the role of frequency (100 Hz-15 MHz) and temperature (from ambient temperature up to 90 degrees C) on the complex effective permittivity which describes the linear response of the system to an electromagnetic wave, we investigate these composites with CB loadings below the percolation threshold. Two features are observed. First, our observations cannot be understood in the typical framework of a simple Debye-like dipolar process. In this analysis, we argue that the appearance of the broad temperature and frequency dependent maximum loss can be understood within the heuristic framework proposed by Jonscher which applies to disordered heterogeneous systems. This theoretical framework is consistent with several aspects of the experiments, notably the power-law decays of the real and imaginary parts of the effective permittivity characterized by two fractional exponents m and n. These exponents are both positive and smaller than unity. We further quantified their different temperature variations: while m is strongly decreasing with increasing temperature, n takes a value close to 1. Second, the observed maximum loss frequency found for each CB volume fraction shifts to higher frequencies with increasing temperature and exhibits a non-Arrhenius temperature dependence well represented by a Vogel-Tammam-Fulcher (VTF) fit. Well below the percolation threshold, the associated activation energy and ordering temperature of the VTF fit are not significantly sensitive upon the CB concentration. Such results are compared to previous related work. (c) 2009 American Institute of Physics. [DOI: 10.1063/1.3149702]