Ultra-sensitive amplitude engineering and sign reversal of circular dichroism in quasi-3D chiral nanostructures.

Abstract

Circular dichroism (CD), as one of the most representative chiroptical effects, provides a simple strategy for the detection and characterization of the molecular chirality. The enhancement and sign reversal of CD are of great importance for its practical applications in chiral bio-sensing, chirality switching and optical filtering, etc. Here, we realize considerable adjustments and the sign reversal of CD in quasi-three-dimensional (quasi-3D) combined Archimedean spiral nanostructures. With special local and lattice configurations, the nanostructures have both right-handed and left-handed geometric chirality, which are designed based on the proximity effect of stencil lithography. We find that the CD response of the nanostructures becomes obvious once its height exceeds 200 nm and can be adjusted by the further increase of the height or the change of the blade spacing of the nanostructures. The CD reversal is achieved by utilizing the competition of two chiral centers when the height or blade spacing exceeds a critical value. Further analysis of the scattering power of multipole moments reveals that the CD modulation is determined by both magnetic dipole moment and electric quadrupole moment. Benefiting from the highly sensitive CD response to the height, the extreme sign reversal of CD is achieved when a sub-10-nm ultrathin medium layer is anchored on the surface of the nanostructures, which provides a promising strategy for ultra-sensitive chiral bio-sensing.