No abstract

2D monolayers represent some of the most deformable inorganic materials, with bending stiffnesses approaching those of lipid bilayers. Achieving 2D heterostructures with similar properties would enable a new class of deformable devices orders of magnitude softer than conventional thin‐film electronics. Here, by systematically introducing low‐friction twisted or heterointerfaces, interfacial engineering is leveraged to tailor the bending stiffness of 2D heterostructures over several hundred percent. A bending model is developed and experimentally validated to predict and design the deformability of 2D heterostructures and how it evolves with the composition of the stack, the atomic arrangements at the interfaces, and the geometry of the structure. Notably, when each atomic layer is separated by heterointerfaces, the total bending stiffness reaches a theoretical minimum, equal to the sum of the constituent layers regardless of scale of deformation—lending the extreme deformability of 2D monolayers to device‐compatible multilayers.

The creation and movement of dislocations determine the nonlinear mechanics of materials. At the nanoscale, the number of dislocations in structures become countable, and even single defects impact material properties. While the impact of solitons on electronic properties is well studied, the impact of solitons on mechanics is less understood. In this study, we construct nanoelectromechanical drumhead resonators from Bernal stacked bilayer graphene and observe stochastic jumps in frequency. Similar frequency jumps occur in few-layer but not twisted bilayer or monolayer graphene. Using atomistic simulations, we show that the measured shifts are a result of changes in stress due to the creation and annihilation of individual solitons. We develop a simple model relating the magnitude of the stress induced by soliton dynamics across length scales, ranging from <0.01 N/m for the measured 5 μm diameter to ∼1.2 N/m for the 38.7 nm simulations. These results demonstrate the sensitivity of 2D resonators are sufficient to probe the nonlinear mechanics of single dislocations in an atomic membrane and provide a model to understand the interfacial mechanics of different kinds of van der Waals structures under stress, which is important to many emerging applications such as engineering quantum states through electromechanical manipulation and mechanical devices like highly tunable nanoelectromechanical systems, stretchable electronics, and origami nanomachines.

Crystalline films offer various physical properties based on the modulation of their thicknesses and atomic structures. The layer-by-layer assembly of atomically thin crystals provides a powerful means to arbitrarily design films at the atomic level, which are unattainable with existing growth technologies. However, atomically clean assembly of the materials with high scalability and reproducibility remains challenging. We report programmed crystal assembly of graphene and monolayer hexagonal boron nitride, assisted by van der Waals interactions, to form wafer-scale films of pristine interfaces with near-unity yield. The atomic configurations of the films are tailored with layer-resolved compositions and in-plane crystalline orientations. We demonstrate batch-fabricated tunnel device arrays with modulation of the resistance over orders of magnitude by thickness control of the hexagonal boron nitride barrier with single-atom precision and large-scale, twisted multilayer graphene with programmable electronic band structures and crystal symmetries. Our results constitute an important development in the artificial design of large-scale films.

The low bending stiffness of atomic membranes from van der Waals ferroelectrics such as α-In2Se3 allow access to a regime of strong coupling between electrical polarization and mechanical deformation at extremely high strain gradients and nanoscale curvatures. Here, we investigate the atomic structure and polarization at bends in multilayer α-In2Se3 at high curvatures down to 0.3 nm utilizing atomic-resolution scanning transmission electron microscopy, density functional theory, and piezoelectric force microscopy. We find that bent α-In2Se3 produces two classes of structures: arcs, which form at bending angles below ∼33°, and kinks, which form above ∼33°. While arcs preserve the original polarization of the material, kinks contain ferroelectric domain walls that reverse the out-of-plane polarization. We show that these kinks stabilize ferroelectric domains that can be extremely small, down to 2 atoms or ∼4 Å wide at their narrowest point. Using DFT modeling and the theory of geometrically necessary disclinations, we derive conditions for the formation of kink-induced ferroelectric domain boundaries. Finally, we demonstrate direct control over the ferroelectric polarization using templated substrates to induce patterned micro- and nanoscale ferroelectric domains with alternating polarization. Our results describe the electromechanical coupling of α-In2Se3 at the highest limits of curvature and demonstrate a strategy for nanoscale ferroelectric domain patterning.