Full Symmetry-Breaking of Electronic and Nuclear Dynamics for Low-Attosecond Resolution of Electronic Chirality

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 nonionizing ultrafast circularly polarized laser pulses at the highest time resolution to date, by 2 orders of magnitude (3.87 attoseconds), of the continuously valued S and R electronic chirality assignments. We partner with 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 afterward. 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).