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

Abstract: Attosecond science is an emerging topic where chirality plays a central role. Here we demonstrate that subjecting iodoacetylene,a geometrically achiral molecule, to a pair of simulated non-ionizing ultrafast circularly polarized laser pulses induces the fastest reversals of the continuously-valued S and R electronic chirality assignments to date, by two orders of magnitude (3.87 attoseconds). 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).