Ultrabroadband Optical Superchirality in a 3D Stacked‐Patch Plasmonic Metamaterial Designed by Two‐Step Glancing Angle Deposition

Low‐cost and large‐scale fabrication of 3D chiral metamaterials is highly desired for potential applications such as nanophotonics devices and chiral biosensors. One of the promising fabrication methods is to use glancing angle deposition (GLAD) of metal on self‐assembled dielectric microsphere array. However, structural handedness varies locally due to long‐range disorder of the array and therefore large‐scale realization of the same handedness is impossible. Here, using symmetry considerations a two‐step GLAD process is proposed to eliminate this longstanding problem. In the proposed scheme, the unavoidable long‐range disorder gives rise to microscale domains of the same handedness but of slightly different structural geometries and ultimately contributes to a broad‐band response. Experimentally, a record‐breaking superchiral response of circular dichroism signal of ≈11° is demonstrated and an average polarization rotation angle of 27° in the visible region on ≈1 cm² sample is observed. Computer‐aided geometric reconstruction with experimental parameters unambiguously reveal the presence of strong structural anisotropy and chirality in the prepared stacked‐patch plasmonic chiral metamaterial; microscopic spectral analyses combined with full‐wave electromagnetic simulations coherently provide deeper insights into the measured circular dichroism and optical activity. The observed chiroptical response can also be flexibly controlled by adjusting the deposition parameters for various potential applications.