Full symmetry-breaking of electronic and nuclear dynamics for low attosecond resolution of electronic chirality

TL;DR

This paper demonstrates the highest time-resolution simulation of electronic and nuclear dynamics in a molecule subjected to ultrafast circularly polarized laser pulses, revealing detailed symmetry-breaking phenomena relevant to chiral science.

Contribution

It introduces a novel simulation approach combining full symmetry-breaking of electronic and nuclear dynamics with ultrafast laser pulses, achieving attosecond resolution without relying on charge density differences.

Findings

Achieved 3.87 attosecond resolution in simulating chiral dynamics.

Quantified 'easy' and 'hard' charge density motion directions.

Revealed cardioid-like and toroidal charge density morphologies during pulses.

Abstract

Attosecond science is an emerging topic where chirality plays a central role. Here we demonstrate subjecting iodoacetylene, a geometrically achiral molecule, to a pair of simulated non-ionizing ultrafast circularly polarized laser pulses at the highest time resolution to date, by two orders of magnitude (3.87 attoseconds), of the continuously-valued S and R electronic chirality assignments. We partner the only vector-based quantum chemical physics theory enabling full symmetry-breaking with electronic and nuclear dynamics simulations: the former does not require charge density differences or special symmetry positions. The resulting 'easy' and 'hard' directions of the total electronic charge density motion are quantified as a cardioid-like morphology for the duration of the simulated laser pulses and toroidal afterwards. Future research directions include determination of the underlying mechanism governing chiral induced spin selectivity, in addition to application to chiral spin selective phenomena in opto-spintronics and exotic superconductors, partnered with orbital-free density functional theory (OF-DFT).