Selective Excitation of Bloch Modes in Canalized Polaritonic Crystals

Abstract Polaritonic crystals (PoCs) have experienced significant advancements through involving hyperbolic polaritons in anisotropic materials such as α‐MoO₃, offering a promising approach for nanoscale light control and improved light‐matter interactions. Notably, twisted bilayer α‐MoO₃ enables tunable iso‐frequency contours (IFCs), especially generating flat IFCs at certain twist angles, which can enhance mode selectivity in their PoCs through the highly collimated and canalized polaritons. This study unveils the selective excitation of Bloch modes in canalized PoCs with square‐lattice structures on twisted bilayer α‐MoO₃. Through the optimization of the square‐lattice design, there is an effective redistribution of canalized polaritons into the reciprocal lattices of PoCs. Fine‐tuning the periodicity and orientation of the hole lattice enables momentum matching between flat IFCs and co‐linear reciprocal points, allowing precise and directional control over desired Bragg resonances and Bloch modes. This research establishes a versatile platform for tunable polaritonic devices and paves the way for advanced photonic applications.