Yuan Hou

Frenkel's cohesive model predicts an ideal elastic strain limit of ~10% for strong solids, a bound upheld in conventional materials. We demonstrate that such consistency breaks down in van der Waals (vdW) solids, challenging established strength theories. In situ tensile tests, combined with first-principles calculations, reveal unexpected localized decohesion failure at only ~3% strain in graphite and ~2% in h-BN along the interlayer direction-well below defect-controlled limits-defining their intrinsic elastic limits. This localization phenomenon is absent in MoS₂, GaSe, and 3D crystals. We identify flexural phonon instability as the trigger for a cascade of strain localization, creating periodic nanogaps to release elastic strain energy. This dynamic instability redefines the intrinsic elastic limits of vdW crystals and opens pathways to tailor their structural/transport properties via strain engineering.

Hexagonal boron nitride (h-BN) has excellent thermal conductivity and dielectric properties, which shows great potential for low-dimensional devices. However, mechanical properties of h-BN have not been comprehensively investigated through experiments. In this work, we conduct in situ direct tensile tests on freestanding single-crystal few-layer h-BN nanosheets with various layer numbers from 3 to 8, with an elaborate sample transfer and characterization protocol. Young's modulus of 573.8 ± 101.4 GPa and a tensile fracture strain up to 3.2% are revealed, which are comparable to its monolayer counterpart. Moreover, we find a tough-to-brittle transition in few-layer h-BN with the increase in layer number, which is attributed the interplay between the van der Waals interaction and in-plane covalent bonding. These findings could open up new possibilities in mechanical research of van der Waals materials and provide guidance for the design of h-BN-based devices and composites.

Conventionally, tuning materials’ properties can be done through strategies such as alloying, doping, defect engineering, and phase engineering, while in fact mechanical straining can be another effective approach. In particular, elastic strain engineering (ESE), unlike conventional strain engineering mainly based on epitaxial growth, allows for continuous and reversible modulation of material properties by mechanical loading/unloading. The exceptional intrinsic mechanical properties (including elasticity and strength) of two-dimensional (2D) materials make them naturally attractive candidates for potential ESE applications. Here, we demonstrated that using the strain effect to modulate the physical and chemical properties toward novel functional device applications, which could be a general strategy for various 2D materials and their heterostructures. We then show how ultralarge, uniform elastic strain in free-standing 2D monolayers can permit deep elastic strain engineering (DESE), which can result in fundamentally changed electronic and optoelectronic properties for unconventional device applications. In addition to monolayers and van der Waals (vdW) heterostructures, we propose that DESE can be also applied to twisted bilayer graphene and other emerging twisted vdW structures, allowing for unprecedented functional 2D material applications.

Assembling monolayers into a bilayer system unlocks the rotational free degree of van der Waals (vdW) homo/heterostructure, which enables the building of twisted bilayer graphene (tBLG) that possesses novel electronic, optical and mechanical properties. Previous methods for preparation of homo/heterstructures inevitably leave the polymer residues or hexagonal boron nitride (h-BN) mask, which usually obstruct the measurement of intrinsic mechanical and surface properties of tBLG. Undoubtedly, to fabricate the designable tBLG with clean interface and surface is necessary but challenging. Here, we propose a simple and handy method to prepare atomically clean twisted bilayer graphene with controllable twist angles based on wetting-induced delamination. This method can transfer tBLG onto the patterned substrate, which offers an excellent platform for the observation of physical phenomena such as relaxation of moiré pattern in marginally tBLG. These findings and insight should ultimately guide the designable packaging and atomic characterization the two-dimensional (2D) materials.

Graphene grown on Cu by chemical vapor deposition is rough due to the surface roughening of Cu for releasing interfacial thermal stress and/or graphene bending energy. The roughness degrades the electrical conductance and mechanical strength of graphene. Here, by using vicinal Cu(111) and flat Cu(111) as model substrates, we investigated the critical role of original surface topography on the surface deformation of Cu covered by graphene. We demonstrated that terrace steps on vicinal Cu(111) dominate the formation of step bunches (SB). Atomically flat graphene with roughness down to 0.2 nm was grown on flat Cu(111) films. By avoiding SB-induced ripples, as-grown ultra-flat graphene maintained its flat feature after transfer. The ultra-flat graphene exhibited extraordinary mechanical properties with Young’s modulus ~ 940 GPa and strength ~ 117 GPa, comparable to mechanical exfoliated ones. Molecular dynamics simulation revealed the mechanism of softened elastic response and weakened strength of graphene with rippled structures.