Moir\'e Engineering in 2D Heterostructures with Process-Induced Strain

We report deterministic control over moir\'e 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 x film thickness) and patterned stressor geometry, respectively. We examine strain and moir\'e interference with Raman spectroscopy through in-plane and moir\'e-activated phonon mode shifts. Results support systematic C$_{3}$ rotational symmetry breaking and tunable periodicity in moir\'e 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 to not only tune moir\'e interference without additional twisting, but also allows for a systematic pathway to explore different van der Waals based moir\'e superlattice symmetries by deterministic design.