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

TL;DR

This paper demonstrates how synthetic chiral light can be used to ultrafastly and sensitively image and control chiral nuclear dynamics during chemical reactions, enabling new insights into enantioselective processes.

Contribution

It introduces a method to probe chiral nuclear rearrangements using nonlinear optical responses driven by synthetic chiral light, advancing ultrafast enantio-sensitive imaging techniques.

Findings

Nonlinear response of H2O2 varies with dihedral angle.

Macroscopic harmonic emission depends on nuclear geometry.

Ultrafast mapping of chiral nuclear dynamics is possible.

Abstract

The recently introduced synthetic chiral light [D. Ayuso et al, Nat. Photon. 13, 866-871 (2019)] 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 an highly enantio-sensitive manner. Using a state-of-the-art implementation of time-dependent density functional theory, we explore how the nonlinear response of the prototypical chiral molecule H2O2 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 chiral dichroism and 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.