Bulletin of the American Physical Society
APS March Meeting 2022
Volume 67, Number 3
Monday–Friday, March 14–18, 2022; Chicago
Session M27: Ultrafast Dynamics and Control of Quantum Materials II
8:00 AM–10:48 AM,
Wednesday, March 16, 2022
Room: McCormick Place W-187C
Sponsoring
Unit:
DLS
Chair: Emroz Khan, Purdue University
Abstract: M27.00003 : Opportunities for imaging chiral nuclear dynamics on ultrafast timescales with synthetic chiral light
8:24 AM–8:36 AM
Presenter:
David Ayuso
(Imperial College London)
Authors:
David Ayuso
(Imperial College London)
Misha Ivanov
(Max-Born-Institut)
Olga Smirnova
(Max-Born-Institut)
The recently introduced 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 a circularly polarized wave. 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 to realize a chiral version of Young’s 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)
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