Geometry‐Dependent Adhesion in Transparent Monodomain Liquid Crystal Elastomers

ABSTRACT Elastomeric pressure‐sensitive adhesives (PSAs) form adhesive bonds under light pressure. Liquid crystal elastomers (LCEs) are exciting PSA candidates as they can impart both anisotropy and temperature‐dependence to adhesion, but the full potential of their anisotropic adhesion is unexplored. Here, identical side‐chain LCEs, produced as transparent isotropic or nematic films, are investigated; the latter aligned in homeotropic or planar geometries. Their room‐temperature adhesion, determined through a 90˚ peel test, is consistent with theoretical predictions and strongest in a planar geometry (peeled parallel to the director) with adhesive force per unit length of 0.067 × 10− 3 Nm −1 . In contrast, adhesion of the planar perpendicular, isotropic, and homeotropic films is 62.5%, 38.5%, and 23.0% lower, respectively. The surface contribution to adhesion is identical for all films, confirming that the variation in adhesion is determined solely by the bulk LCE alignment controlled during film preparation. A temperature‐dependent adhesion factor is determined from 0˚C to 80˚C using dynamic mechanical analysis, and found to be in excellent agreement with the peel data at room temperature. Molecular relaxations active above the glass transition temperature are dominant in determining LCE adhesion. The results show that side‐chain LCEs can function as transparent, tunable, broad‐temperature smart PSAs.