Crystal
engineering of temporary adhesion is important in diverse
fields ranging from healthcare to manufacturing. Molecular solidsa
broad class of crystalline materials characterized by discrete molecules
with well-defined chemical and crystal structurescan be utilized
as sublimable adhesives to achieve rapid adhesion, strong mechanical
bonding, and facile on-demand release of surfaces. Through systematic
investigation of the interfacial and bulk properties of molecular
solids, this paper shows that this class of materials can exhibit
remarkable mechanical strength (resistance to shear stress up to 2100
kPa and shear strain up to 37, as well as shear moduli up to 1000
kPa) yet enable on-demand (within minutes) release from adhesion through
controlled sublimation without the application of solvents and/or
mechanical force. Intermolecular interactions heavily influence the
mechanical performance via preferential orientation of the solid relative
to surfaces during the melt-bonding process. This research quantifies
how chemical and crystal structures inform macroscopic mechanical
properties of polycrystalline solids.