The sp² nature of graphene endows the hexagonal lattice with very high theoretical stiffness, strength and resilience, all well-documented. However, the ultimate stretchability of graphene has not yet been demonstrated due to the difficulties in experimental design. Here, directly performing in situ tensile tests in a scanning electron microscope after developing a protocol for sample transfer, shaping and straining, we report the elastic properties and stretchability of free-standing single-crystalline monolayer graphene grown by chemical vapor deposition. The measured Young’s modulus is close to 1 TPa, aligning well with the theoretical value, while the representative engineering tensile strength reaches ~50-60 GPa with sample-wide elastic strain up to ~6%. Our findings demonstrate that single-crystalline monolayer graphene can indeed display near ideal mechanical performance, even in a large area with edge defects, as well as resilience and mechanical robustness that allows for flexible electronics and mechatronics applications.

Out-of-plane deformation patterns, such as buckling, wrinkling, scrolling, and folding, formed by multilayer van der Waals materials have recently seen a surge of interest. One crucial parameter governing these deformations is bending rigidity, on which significant controversy still exists despite extensive research for more than a decade. Here, we report direct measurements of bending rigidity of multilayer graphene, molybdenum disulfide (${\mathrm{MoS}}_2$), and hexagonal boron nitride (hBN) based on pressurized bubbles. By controlling the sample thickness and bubbling deflection, we observe platelike responses of the multilayers and extract both their Young’s modulus and bending rigidity following a nonlinear plate theory. The measured Young’s moduli show good agreement with those reported in the literature ($E_{\text{graphene}}>E_{\text{hBN}}>E_{{\text{MoS}}_2}$), but the bending rigidity follows an opposite trend, $D_{\text{graphene}}<D_{\text{hBN}}<D_{{\text{MoS}}_2}$ for multilayers with comparable thickness, in contrast to the classical plate theory, which is attributed to the interlayer shear effect in the van der Waals materials.

Monolayer two-dimensional (2D) crystals exhibit a host of intriguing properties, but the most exciting applications may come from stacking them into multilayer structures. Interlayer and interfacial shear interactions could play a crucial role in the performance and reliability of these applications, but little is known about the key parameters controlling shear deformation across the layers and interfaces between 2D materials. Herein, we report the first measurement of the interlayer shear stress of bilayer graphene based on pressurized microscale bubble loading devices. We demonstrate continuous growth of an interlayer shear zone outside the bubble edge and extract an interlayer shear stress of 40 kPa based on a membrane analysis for bilayer graphene bubbles. Meanwhile, a much higher interfacial shear stress of 1.64 MPa was determined for monolayer graphene on a silicon oxide substrate. Our results not only provide insights into the interfacial shear responses of the thinnest structures possible, but also establish an experimental method for characterizing the fundamental interlayer shear properties of the emerging 2D materials for potential applications in multilayer systems.