Multi Moire Networks in Engineered Lateral Hetero-Bilayers: Programmable Phononic Reconfiguration and Second Harmonic Generation

Abstract: Moire engineering in two-dimensional transition metal dichalcogenides enables access to correlated quantum phenomena. Realizing such effects demands simultaneous control over twist angle and material composition to modulate phonons, excitons, and their interactions. However, most studies rely on exfoliated flakes, limiting scalability and systematic exploration. Here, we demonstrate a scalable multi-moire network by vertically stacking CVD-grown monolayer lateral heterostructures. Signatures of moire non-rigidity, including phonon frequency softening, linewidth broadening, and strain localization, are attributed to two lattice relaxation modes; rotational reconstruction and volumetric dilation. Micro-angle-resolved photoemission spectroscopy reveals that interfacial orbital interactions modulate interlayer coupling. At aligned angles, molybdenum diselenides exhibit reduced valley polarization and Davydov splitting, indicating strain-induced symmetry breaking and chiral phonon effects. Notably, SHG modulation was obderved with variation in twist angle due to lower coherence and band-offset-driven phase delay. First-principles calculations support these findings. This work provides a route to programmable, scalable multi-moire platforms for opto-straintronics, quantum sensing, and on-chip photonics.