Bulletin of the American Physical Society
53rd Annual Meeting of the APS Division of Atomic, Molecular and Optical Physics
Volume 67, Number 7
Monday–Friday, May 30–June 3 2022; Orlando, Florida
Session U07: Chiral Matter and Chiral Light
2:00 PM–3:48 PM,
Thursday, June 2, 2022
Room: Salon 5/6
Chair: Loren Greenman, Kansas State
Abstract: U07.00002 : New opportunities for imaging chiral nuclear dynamics in chiral molecules on ultrafast time scales with synthetic chiral light
2:12 PM–2:24 PM
Presenter:
David Ayuso
(Imperial College London)
Author:
David Ayuso
(Imperial College London)
Synthetic chiral light [2,3] allows us to bypass this fundamental limitation by encoding chirality in time, rather than relying on the spatial helix of circularly polarized light. Such light is locally chiral: the tip of the electric-field vector draws a chiral (3D) Lissajous figure in time, at every point in space. It produces giant enantio-sensitivity (100%) at the level of total intensity signals [2]. We have also shown that light's local handedness can be structured in space to realize a chiral double-slit experiment that leads to enantio-sensitive light bending [3].
Here we show how to exploit the giant enantio-sensitivity enabled by synthetic chiral light to probe chiral nuclear rearrangements during chemical reactions in a highly enantio-sensitive manner. Using 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 direct mapping between chiral dichroism and nuclear geometry provides a way of probing chiral nuclear dynamics at their natural time scales. Our work paves the way for ultrafast and highly efficient imaging of enantio-sensitive dynamics in complex chiral systems, including biologically relevant molecules.
[1] Berova et al, Comprehensive Chiroptical Spectroscopy (Wiley, 2013)
[2] Ayuso et al, Nat Photon 13, 866 (2019)
[3] Ayuso et al, Nat Commun 12, 3951 (2021)
[4] Ayuso, arXiv:2111.13671 (2021)
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