“…[1] Beyond conventional techniques, including DOI: 10.1002/adom.202302407 doping, [2] chemical modification, [3] and electrostatic control, [4] augmenting material performance, an innovative avenue, arises through the manipulation of the relative layer twist, introducing a critical new dimension for the design of stacked structures endowed with emergent functionalities. [5,6] The variation in the twist angle between the layers serves to finely modulate not only the energyband architecture but also the overall symmetry of the system. This dual influence is of paramount importance in a wide range of physical processes, including linear optical phenomena such as photoluminescence (PL), [7,8] Raman [9,10] and nonlinear optical behaviors, including nonlinear absorption, [11] and second-harmonic generation (SHG).…”