Engineering the Dipole Orientation and Symmetry Breaking with Mixed‐Dimensional Heterostructures

Engineering of the dipole and the symmetry of materials plays an important role in fundamental research and technical applications. Here, a novel morphological manipulation strategy to engineer the dipole orientation and symmetry of 2D layered materials by integrating them with 1D nanowires (NWs) is reported. This 2D InSe –1D AlGaAs NW heterostructure example shows that the in‐plane dipole moments in InSe can be engineered in the mixed‐dimensional heterostructure to significantly enhance linear and nonlinear optical responses (e.g., photoluminescence, Raman, and second harmonic generation) with an enhancement factor of up to ≈12. Further, the 1D NW can break the threefold rotational symmetry of 2D InSe, leading to a strong optical anisotropy of up to ≈65%. These results of engineering dipole orientation and symmetry breaking with the mixed‐dimensional heterostructures open a new path for photonic and optoelectronic applications.