Engineering a strong and stable ultraviolet chiroptical effect in a large-area chiral plasmonic shell.

Ultraviolet chiral metamaterials (UCM) are highly desired for their strong interaction with the intrinsic resonance of molecules and ability in manipulating the polarization state of high energy photons, but rarely reported to date due to their small feature size and complex geometry. Herein, we design and fabricate a kind of novel ultraviolet chiral plasmonic shell (UCPS) by combing the stepwise Al deposition and colloid-sphere assembled techniques. The cancellation effect originated from the disorder lattices of micro-domains in the colloid monolayer has been successfully overcome by optimizing the deposition parameters, and a strong CD signal of larger than 1 deg in the UV region is demonstrated both in simulation and experiment. This strong ultraviolet chiroptical resonances mainly come from the surface chiral lattice resonance mode, the whispering gallery mode and also the interaction between neighbor shells, and can be effectively tuned by changing structural parameters, for example, the sphere diameter, or even slightly increasing the deposition temperature in experiment. To improve the stability, the fabricated UCPSs are protected by N in the deposition chamber and then passivated by UV-ozone immediately after each deposition step. The formed UCPS show an excellent stability when exposing in the atmospheric environment. The computer-aided geometrical model, electromagnetic modes, and the tunable chiroptical resonance modes have been systematically investigated.