Relaxation Phenomena in Chitosan-Au Nanoparticle Thin Films

Chitosan-gold nanoparticle (CS/AuNP) thin films were synthesized through the chemical reduction of HAuCl₄ in sodium citrate/chitosan solutions. The dielectric and dynamic mechanical behaviors of CS/AuNP films have been investigated as a function of moisture and HAuCl₄ content. Two relaxation processes in the nanocomposites have been observed. The α-relaxation process is related to a glass transition in wet CS/AuNP films. However, in dry composites (with 0.2 wt% of moisture content), the glass transition vanished. A second relaxation process was observed from 70 °C to the onset of thermal degradation (160 °C) in wet films and from 33 °C to the onset of degradation in dry films. This relaxation is identified as the σ-relaxation and may be related to the local diffusion process of ions between high potential barriers in disordered systems. The α- and σ-relaxation processes are affected by the HAuCl₄ content of the solutions from which films were obtained because of the interaction between CS, sodium succinate, and gold nanoparticles. With about 0.6 mM of HAuCl₄, the conductivity of both wet and dry films sharply increased by six orders, corresponding to the percolation effect, which may be related to the appearance of a conductivity pathway between AuNPs, HAuCl₄, and NaCl.