Structuring the local handedness of synthetic chiral light: global chirality versus polarization of chirality

Abstract

Synthetic chiral light enables ultrafast and highly efficient imaging of molecular chirality. Unlike standard circularly polarized light, the handedness of synthetic chiral light does not rely on the spatial structure of the light field: it is encoded locally, in the chiral trajectory that the tip of the electric-field vector draws in time, at each point in space. Synthetic chiral light that is both locally and globally chiral (Ayuso et al 2019 Nat. Photon. 13 866) allows us to selectively quench the nonlinear response of a selected molecular enantiomer while maximizing it in its mirror twin at the level of total signal intensities. Synthetic chiral light that exhibits polarization of chirality (Ayuso et al 2021 Nat. Commun. 12 3951) allows us to realize a chiral version of Young’s double-slit experiment that leads to enantio-sensitive light bending. Here we connect these new concepts, and show how one can structure the local and global handedness of synthetic chiral light in space to create optical fields which can be both globally chiral and chirality polarized. Using state-of-the-art computational modeling, we show how these local and global properties are imprinted in the enantio-sensitive response of chiral molecules, creating exciting opportunities for ultrafast, all-optical and highly efficient imaging of molecular chirality.