arXiv:2508.19519v1 Announce Type: new
Abstract: The spin dynamics of electrons in chiral molecular systems remains a topic of intense interest, particularly regarding whether geometric chirality inherently induces spin polarization or simply modulates spin transport. In this work, we employ ab initio real-time time-dependent density functional theory (rt-TDDFT) to directly simulate the interplay between charge current, spin, and orbital. This real-time tracking goes beyond perturbative treatments, and we analyze how nonequilibrium currents effectively lift the symmetry constraints of screw-rotation and time-reversal symmetry. We find that above a critical current threshold, time-reversal symmetry constraints are dynamically lifted — leading to pronounced spin and orbital polarizations, even when the underlying Hamiltonian remains symmetric. Notably, the emergence of spin and orbital angular momenta dynamics correlates with a loss of translational (linear) momentum, suggesting a redistribution of angular degrees of freedom as an intrinsic consequence of a current-driven symmetry lowering in a chiral system, with implications for chirality-induced spin selectivity and spintronic device design.