Dzyaloshinskii-Moriya interaction as a coherence diagnostic for chirality-induced spin selectivity

Original Abstract

Whether chirality-induced spin selectivity (CISS) reflects coherent SU(2) spin rotation or incoherent spin-dependent filtering is a central unresolved question in molecular spintronics, with implications ranging from asymmetric chemistry to quantum information. We show that these two scenarios are distinguishable by a sharp symmetry criterion on the superexchange interaction mediated by a chiral molecular bridge. Coherent CISS, implemented as a unitary spin rotation of the tunneling electron, generates a giant Dzyaloshinskii-Moriya (DM) interaction with ratio |D|/JH up to 3, which is two orders of magnitude beyond intrinsic Rashba spin-orbit coupling in Si/SiGe. Incoherent CISS, represented by any Hermitian (non-unitary but spin-diagonal) tunneling matrix, produces D = 0 identically; we prove this as a structural theorem, reinforced by a Lindblad argument that dissipative spin filtering cannot modify virtual-tunneling-mediated superexchange. The DM interaction thus serves as a coherence order parameter, nonzero only when quantum amplitudes for opposite-spin transmission maintain a fixed relative phase. We derive closed-form angular, enantiomeric, and sensitivity signatures and show that the critical coherent rotation angle lies two orders of magnitude below current transport-inferred values and is accessible to existing 10 kHz exchange spectroscopy in gate-defined quantum dots. Five candidate molecules are predicted to exceed this threshold by one to two orders of magnitude even in a conservative interface-amplification scenario. The proposed measurement converts a long-standing transport controversy into a binary spin-qubit experiment with quantum-amplitude resolution.