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The recently introduced synthetic chiral light [D. Ayuso et al, Nat. Photon.13, 866-871 (2019)] has opened up new opportunities for ultrafast and highlyefficient imaging and control of chiral matter. Here we show that the giantenantio-sensitivity enabled by such light could be exploited to probe chiralnuclear rearrangements during chemical reactions in an highly enantio-sensitivemanner. Using a state-of-the-art implementation of time-dependent densityfunctional theory, we explore how the nonlinear response of the prototypicalchiral molecule H2O2 changes as a function of its dihedral angle, which definesits handedness. The macroscopic intensity emitted from randomly orientedmolecules at even harmonic frequencies (of the fundamental) depends strongly onthis nuclear coordinate. Because of the ultrafast nature of such nonlinearinteractions, the direct mapping between chiral dichroism and nuclear geometryprovides a way to probe chiral nuclear dynamics at their natural time scales.Our work paves the way for ultrafast and highly efficient imaging ofenantio-sensitive dynamics in more complex chiral systems, includingbiologically relevant molecules.

New opportunities for ultrafast and highly enantio-sensitive imaging and control of chiral nuclear dynamics: towards enantio-selective attochemistry