Mechanical Characterization of Stacked Single‐Crystal of Polyethylene and Monolayer MoSe₂

Abstract Polymer single crystal (SC) is a key building block of semicrystalline polymers. However, direct experimental measurement of freestanding mono‐lamella polymer SC has not been demonstrated. This is, in large part, due to the difficulties associated with manipulating freestanding individual mono‐lamella SC because of its extremely low rigidity and low robustness. Here, we demonstrate a new strategy to successfully suspend and test a polymer SC by using a 2D material as backing. In particular, mono‐lamella polyethylene (PE) SC is stacked on monolayer MoSe₂, and the hybrid stacks can be suspended over microholes. Nanoindentation is used to probe the suspended PE‐SC/MoSe₂ stacks and MoSe₂ monolayers. The results suggest the first experimentally‐measured in‐plane moduli of PE‐SC and 2D MoSe₂ as 32 ± 3 and 237 ± 15 GPa, respectively. Such a stacked unit represents an ultrathin structure of polymer‐ceramic laminate and the idea can be applied to other laminated composite systems. Therefore, this research will pave the way to accurately measure the mechanical properties of polymer SCs and their composites, as well as provide a key insight on designing composite structures.