New opportunities for ultrafast and highly enantio-sensitive imaging of chiral nuclear dynamics enabled by synthetic chiral light.

Synthetic chiral light [D. Ayuso et al. , Nat. Photon. , 2019, 13 , 866-871] has opened up new opportunities for ultrafast and highly efficient imaging and control of chiral matter. Here we show that the giant enantio-sensitivity enabled by such light could be exploited to probe chiral nuclear rearrangements during chemical reactions in a highly enantio-sensitive manner. Using a state-of-the-art implementation of real-time time-dependent density functional theory, we explore how the nonlinear response of the prototypical chiral molecule H 2 O 2 changes as a function of its dihedral angle, which defines its handedness. The macroscopic intensity emitted from randomly oriented molecules at even harmonic frequencies (of the fundamental) depends strongly on this nuclear coordinate. Because of the ultrafast nature of such nonlinear interactions, the direct mapping between the dissymmetry factor and the nuclear geometry provides a way to probe chiral nuclear dynamics at their natural time scales. Our work paves the way for ultrafast and highly efficient imaging of enantio-sensitive dynamics in more complex chiral systems, including biologically relevant molecules.