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We report a method of engineering a reversible change in interlayer bonding between layers of exfoliated thin films of MoS2 by means of hydrogen intercalation through forming gas annealing. Interlayer bonding strength is probed through the behavior of MoS2 under process-induced strain engineering, where two-dimensional (2D) flakes are encapsulated with a deposited stressed thin film layer to transfer strain into the underlying 2D materials. It is shown that after forming gas annealing, the depth of the strain transferred into multilayer MoS2 is enhanced as determined through layer-thickness-dependent Raman spectroscopic mapping. This change represents a transition from a 2D van der Waals-bonded material in the as-exfoliated samples to a more three-dimensional (3D)-bonded system in the annealed samples. We demonstrate the reversibility of this effect by means of vacuum annealing of previously forming gas annealed samples. The process of forming gas annealing itself also imparts strain into MoS2 due to a combination of 2D-to-3D bonding transition with differential thermal mismatch between the MoS2 and the substrate. These strains are shown to be retained after the vacuum annealing process, despite the transition back to 2D bonding. Since forming gas annealing is a common technical process in engineering 2D electronic devices, these results represent an important consideration in understanding non-intentionally applied strains due to changes in the mechanical properties of 2D materials. 

The layer stacking order in two-dimensional heterostructures, like graphene, affects their physical properties and potential applications. Trilayer graphene, specifically ABC-trilayer graphene, has captured significant interest due to its potential for correlated electronic states. However, achieving a stable ABC arrangement is challenging due to its lower thermodynamic stability compared to the more stable ABA stacking. Despite recent advancements in obtaining ABC graphene through external perturbations, such as strain, the stacking transition mechanism remains insufficiently explored. In this study, we unveil a universal mechanism to achieve ABC stacking, applicable for understanding ABA to ABC stacking changes induced by any mechanical perturbations. Our approach is based on a novel strain engineering technique that induces interlayer slippage and results in the formation of stable ABC domains. We investigate the underlying interfacial mechanisms of this stacking change through computational simulations and experiments. Our findings demonstrate a highly anisotropic and significant transformation of ABA stacking to large and stable ABC domains facilitated by interlayer slippage. Through atomistic simulations and local energy analysis, we systematically demonstrate the mechanism for this stacking transition, that is dependent on specific loading orientation. Understanding such a mechanism allows this material system to be engineered by design compatible with industrial techniques on a device-by-device level. We conduct Raman studies to validate and characterize the formed ABC stacking, highlighting its distinct features compared to the ABA region. Our results contribute to a clearer understanding of the stacking change mechanism and provide a robust and controllable method for achieving stable ABC domains, facilitating their use in developing advanced optoelectronic devices. 

Strain engineering in two-dimensional (2D) materials is a powerful but difficult to control approach to tailor material properties. Across applications, there is a need for device-compatible techniques to design strain within 2D materials. This work explores how process-induced strain engineering, commonly used by the semiconductor industry to enhance transistor performance, can be used to pattern complex strain profiles in monolayer MoS2 and 2D heterostructures. A traction–separation model is identified to predict strain profiles and extract the interfacial traction coefficient of 1.3 ± 0.7 MPa/μm and the damage initiation threshold of 16 ± 5 nm. This work demonstrates the utility to (1) spatially pattern the optical band gap with a tuning rate of 91 ± 1 meV/% strain and (2) induce interlayer heterostrain in MoS2–WSe2 heterobilayers. These results provide a CMOS-compatible approach to design complex strain patterns in 2D materials with important applications in 2D heterogeneous integration into CMOS technologies, moiré engineering, and confining quantum systems. 

We demonstrate a technique to strain two-dimensional hexagonal boron nitride (hBN) and graphene by depositing stressed thin films to encapsulate exfoliated flakes. We choose optically transparent stressors to be able to analyze strain in 2D flakes through Raman spectroscopy. Combining thickness-dependent analyses of Raman peak shifts with atomistic simulations of hBN and graphene, we can explore layer-by-layer strain transfer in these materials. hBN and graphene show strain transfer into the top four and two layers of multilayer flakes, respectively. hBN has been widely used as a protective capping layer for other 2D materials, while graphene has been used as a top gate layer in various applications. Findings of this work suggest that straining 2D heterostructures with evaporated stressed thin films through the hBN capping layer or graphene top contact is possible since strain is not limited to a single layer. 

We report deterministic control over a moiré superlattice interference pattern in twisted bilayer graphene by implementing designable device-level heterostrain with process-induced strain engineering, a widely used technique in industrial silicon nanofabrication processes. By depositing stressed thin films onto our twisted bilayer graphene samples, heterostrain magnitude and strain directionality can be controlled by stressor film force (film stress × film thickness) and patterned stressor geometry, respectively. We examine strain and moiré interference with Raman spectroscopy through in-plane and moiré-activated phonon mode shifts. Results support systematic C 3 rotational symmetry breaking and tunable periodicity in moiré superlattices under the application of uniaxial or biaxial heterostrain. Experimental results are validated by molecular statics simulations and density functional theory based first principles calculations. This provides a method not only to tune moiré interference without additional twisting but also to allow for a systematic pathway to explore different van der Waals based moiré superlattice symmetries by deterministic design.