Mechanics of shape-locking-governed R2G adhesion with shape memory polymers

Shape memory polymers (SMPs), with unique properties such as tunable elastic modulus, temporary shape locking and shape recovery upon external stimulation, are emerging as a new class of smart materials with switchable adhesion capabilities. A prominent feature of the adhesion between SMP and a spherical indenter is the so-called R2G adhesion, defined as making contact in the rubbery state to a certain indentation depth followed by detachment in the glassy state. While it has been demonstrated that the R2G adhesion with SMPs can achieve orders of magnitude higher adhesive strength compared to conventional elastic adhesive systems with similar geometrical and adhesion parameters, the fundamental mechanics of R2G adhesion and why it leads to such tremendous adhesion enhancement remain largely mysterious at this point. Here, combined experimental testing, theoretical analysis, and finite element analysis (FEA) based on a thermomechanical constitutive model of SMP are performed to investigate the mechanics of R2G adhesion with a rigid spherical indenter. It is shown that the orders of magnitude enhancement of R2G adhesion over conventional elastic adhesion systems is mostly governed by the shape locking effect during the transition from the rubbery to glassy states. The shape locking effect freezes the deformed configuration of the SMP substrate, resulting in nearly conformal contact between the spherical indenter and the glassy-state SMP substrate, thus greatly increases the effective radius of curvature of the contact surface. Our experimental measurements and FEA analysis demonstrate that the net effect of shape locking leads to a pull-off force of a sphere nearly the same as that of a flat punch on an elastic half-space with the same contact radius. An explicit expression of the pulloff force for R2G adhesion is proposed based on flat-punch adhesion. Our results from combined experimentation, modeling and simulations reveal the fundamental mechanics of R2G adhesion. Such understanding provides guidance for the design of SMP smart adhesives.