Extra-High Mechanical and Phononic Anisotropy in Black Phosphorus Blisters.

Strain is an effective strategy to modulate the electrical, optical, and optoelectronic properties of 2D materials. Conventional circular blisters could generate a biaxial stretching of 2D membranes with notable strain gradients along the hoop direction. However, such a deformation mode cannot be utilized to investigate mechanical responses of in-plane anisotropic 2D materials, for example, black phosphorus (BP), due to its crystallographic orientation dependence. Here, a novel rectangular-shaped bulge device is developed to uniaxially stretch the membrane, and further provide a promising platform to detect orientation-dependent mechanical and optical properties of anisotropic 2D materials. Impressively, the derived anisotropic ratio of Young's modulus of BP flakes is much higher than the values obtained via the nanoindentation method. The extra-high strain-dependent phononic anisotropy in Raman modes along different crystalline orientations is also observed. The designed rectangular budge device expands the uniaxial deformation methods available, allowing to explore the mechanical, and strain-dependent physical properties of other anisotropic 2D materials more broadly.

Elastocapillary cleaning of twisted bilayer graphene interfaces.

Although layered van der Waals (vdW) materials involve vast interface areas that are often subject to contamination, vdW interactions between layers may squeeze interfacial contaminants into nanopockets. More intriguingly, those nanopockets could spontaneously coalesce into larger ones, which are easier to be squeezed out the atomic channels. Such unusual phenomena have been thought of as an Ostwald ripening process that is driven by the capillarity of the confined liquid. The underlying mechanism, however, is unclear as the crucial role played by the sheet's elasticity has not been previously appreciated. Here, we demonstrate the coalescence of separated nanopockets and propose a cleaning mechanism in which both elastic and capillary forces are at play. We elucidate this mechanism in terms of control of the nanopocket morphology and the coalescence of nanopockets via a mechanical stretch. Besides, we demonstrate that bilayer graphene interfaces excel in self-renewal phenomena.

Strain Characterization in Two-Dimensional Crystals.

Two-dimensional (2D) crystals provides a material platform to explore the physics and chemistry at the single-atom scale, where surface characterization techniques can be applied straightforwardly. Recently there have been emerging interests in engineering materials through structural deformation or transformation. The strain field offers crucial information of lattice distortion and phase transformation in the native state or under external perturbation. Example problems with significance in science and engineering include the role of defects and dislocations in modulating material behaviors, and the process of fracture, where remarkable strain is built up in a local region, leading to the breakdown of materials. Strain is well defined in the continuum limit to measure the deformation, which can be alternatively calculated from the arrangement of atoms in discrete lattices through methods such as geometrical phase analysis from transmission electron imaging, bond distortion or virial stress from atomic structures obtained from molecular simulations. In this paper, we assess the accuracy of these methods in quantifying the strain field in 2D crystals through a number of examples, with a focus on their localized features at material imperfections. The sources of errors are discussed, providing a reference for reliable strain mapping.

Pattern Development and Control of Strained Solitons in Graphene Bilayers.

Engineering strain and interlayer registry in 2D crystals have been demonstrated as effective controls of their properties. Separation of domains with different interlayer registries in graphene bilayer has been reported, but the pattern control of strained solitons has not yet been achieved. We show here that, by pulling a graphene bilayer apart, soliton structures with a regularly modulated interlayer registry arise from the competition between elastic deformation in monolayers and local slip at the van der Waals interfaces. The commensurate-incommensurate transition with strain localization is identified as the interlayer overlap exceeds a critical size, where the continuum description of load transfer through the tension-shear chain breaks down. Birth, development and annihilation processes of the strained solitons can be controlled by the loading conditions. The effects of lattice symmetry and mechanical constraints are also discussed, completing the picture for microstructural evolution processes in the homo- or heterostructures of 2D crystals.

How Universal Is the Wetting Aging in 2D Materials.

Previous studies indicate that 2D materials such as graphene, WS2, and MoS2 deposited on oxidized silicon substrate are susceptible to aging due to the adsorption of airborne contamination. As a result, their surfaces become more hydrophobic. However, it is not clear how ubiquitous such a hydrophobization is, and the interplay between the specific adsorbed species and resultant wetting aging remains elusive. Here, we report a pronounced and general hydrophilic-to-hydrophobic wetting aging on 2D InSe films, which is independent of the substrates to synthesize these films (silicon, glass, nickel, copper, aluminum oxide), though the extent of wetting aging is sensitive to the layer of films. Our findings are ascribed to the occurrence and enrichment of airborne contamination that contains alkyl chains. Our results also suggest that the wetting aging effect might be universal to a wide range of 2D materials.

Elastic straining of free-standing monolayer graphene.

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.

Bending of Multilayer van der Waals Materials.

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 (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_{graphene}>E_{hBN}>E_{MoS_{2}}), but the bending rigidity follows an opposite trend, D_{graphene}

Edges facilitate water evaporation through nanoporous graphene.

Understanding molecular processes of evaporation at the liquid-vapor interfaces is of critical importance for development of phase-change-related applications. The interfacial behaviors are defined by liquid-vapor equilibrium following thermodynamic rules, while the process through nanopores can be modulated by spatial confinement and intermolecular interaction with the pore. Based on molecular dynamics simulations, we explore water evaporation across nanoporous graphene membranes, which have been recently fabricated by, for example, ion or beam irradiation. The simulation results suggest that the molecular outflow can be facilitated by the graphene edges, boosting the overall evaporative flux by more than 100%. Free-energy analysis shows that the affinity of the graphene edge for water molecules provides a 'hub'-like function in the path of molecular effusion, reducing the free energy barrier for evaporation across the liquid-vapor interface. This prominent edge effect can be further engineered by modifying the atomic charges. Our findings demonstrate the feasibility of nanoengineering for the liquid-vapor phase-change processes using nanoporous graphene as a model system, which can find applications in heat transfer and energy conversion with high efficiency.