As the family of two−dimensional(2D) materials has grown, two−dimensional heterostructure devices have emerged as great alternatives to replace conventional electronic materials and enable new functionality such as flexible and bendable electronics. The fabrication and performance of these devices depend critically on the understanding and ability to manipulate the mechanical interplay between the stacked materials. In this dissertation, we investigate adhesive interactions and determine the shear modulus of heterostructure devices made from Molybdenum Disulfide (MoS2). MoS2 has been attracting attention recently due to its semiconductor nature (having a direct band gap of 1.9 eV) along with its exceptional mechanical strength and flexibility. As the first step of our research, we suspended MoS2 flakes grown through chemical vapor deposition (CVD) over substrates made of metal (gold, titanium, chromium), semiconductor (germanium, silicon), insulator (silicon oxide), and semi-metal (graphite). Then, by creating pressure differences across the membrane, we forced MoS2 to bulge upward until we observe separation from the surface of the substrates. We demonstrated that MoS2 on graphite has the highest work of separation within the tested surface materials. Furthermore, we measured considerable adhesion hysteresis between the work of separation and the work of adhesion. We proposed that surface roughness and chemical interactions play a role in surface adhesion and separation of 2D materials. These experiments are critical to guiding the future design of electrical and mechanical devices based on 2D materials. Next, we measured the effective shear modulus of MoS2/few−layer graphene (FLG) heterostructures by employing a blister test. Again, by introducing a pressure differential across the suspended MoS2 membrane over the FLG substrate, the MoS2/FLG heterostructure peeled off from the silicon oxide surface once the critical pressure is exceeded. Incorporating a modified free energy model and Hencky’s axisymmetric membrane solution, we determine the average effective shear modulus of the heterostructure. This is the first experimental measurement of the shear modulus of heterostructure devices using a blister test and this platform can be extended to determine the shear modulus of other 2D heterostructures as well. / 2024-05-24T00:00:00Z