Effects of degree of cross-links on adhesion curves of cross-linked polymers observed by a point-contact method.

The effects of degree of cross-links on the adhesion properties of polydimethylsiloxane (PDMS) were investigated with the use of a point-contact method in air at room temperature. The degree of cross-links, rho, was varied in a wide range, inducing changes in the rheology of the cross-linked PDMS from viscous solution to elastic gel, and the adhesion properties were examined by changing the separation velocity under a constant normal load and waiting period prior to separation. As a result, the adhesion force, F(A), strongly depended on rho and showed a maximum at a characteristic rho around the loss tangent (tan delta) = 1. In addition, the shapes of the adhesion curves were found to depend strongly on rho, and they were categorized into four types. The different states of cross-linked polymers, i.e., elastic-gel type, weak-gel type, and solution type, showed the different shapes. In the case of the weak gel, two types of characteristic adhesion curves were obtained, which resulted from the different separation mechanisms with and without cavitations near the surface due to the interface and cohesive failures. In the intermediate range of rho, viscous or elastic fingering was detected, which resulted in the characteristic shape of the adhesion curve. The factors determining the type of the adhesion curves are discussed in terms of the microscopic surface, bulk properties, and the different shapes of the adhesive front at the contact surface.