Quantum Formulation of the Spinterface Model

Abstract

We present a fully quantum formulation of the spinterface model for the chirality-induced spin selectivity (CISS) effect, implemented within the non-equilibrium Green's function (NEGF) formalism. The model consists of a gold atom hosting a localised magnetic moment, coupled to a chiral molecular chain with Rashba spin-orbit coupling, and contacted by two non-magnetic leads. The magnetic moment is determined self-consistently from the non-equilibrium electronic distribution, and the spin-resolved transmission is computed from the mean-field Hamiltonian. We show that the interfacial magnetic moment and the chiral Rashba term cooperate to produce large current polarisations that reproduce the key experimental signatures of CISS: high polarisation, a threshold emergence at four total sites followed by interference-modulated growth with chain length, thermal suppression, and sign reversal upon chirality inversion. The central new result of this work is a clean separation of the CISS effect into an even (achiral) and an odd (chiral) contribution to the spin current, $I_{S_z}(ϕ) = I_{S_z}^{\rm even}(ϕ) + I_{S_z}^{\rm odd}(ϕ)$. We demonstrate that $I_{S_z}^{\rm odd}$ vanishes exactly at fixed $m_z$ for chains of fewer than four sites and becomes non-zero for chains of four or more sites, with the smallest junction exhibiting a non-zero odd part being the four-site geometry (one gold atom plus three molecular sites). The odd part arises from reciprocity breaking in a device that is simultaneously chiral, magnetically asymmetric (moment on the gold end only), and long enough to support two or more Rashba-active bonds. This provides a direct, parameter-free test of whether an observed spin signal is genuinely chiral or arises from an achiral spin-valve mechanism.