Origination of the chiroptical effect in plasmonic nano-structures in the view of quasi-normal mode theory.

Abstract

General chiroptical effects describe all of the interaction differences between light carrying opposite spins and chiral matters, such as circular dichroism, optical activity, and chiral Raman optical activity, and have been proven to hold great promise for extensive applications in physics, chemistry, and biology. However, the underlying physical mechanism is usually explained intangibly by the twisted currents in chiral geometry, where the cross coupling between the electric and magnetic dipoles breaks the degeneracy of the helicity eigenmodes. In this Letter, we construct a clear sight on the origination of the chiroptical effect in the view of the eigenstates of a non-Hermitian system, i.e., quasi-normal modes (QNMs). The intrinsic chiroptical effect comes from the chiral QNMs, which have distinct excitation and emission differences in both phase and intensity for lights carrying opposite spins, while the extrinsic chiroptical effect coming from the achiral QNMs requires specific illumination and observation conditions, where the low symmetrical QNM can generate chiroptical effects in both absorption and scattering, but the highly symmetrical QNMs can only generate chiroptical effects in scattering through the coherent superposition of several QNMs. Our findings offer an in-depth understanding of the chiroptical effect and have the potential to bring broad inspiration to the design and applications of chiroptical effects.