The Spinterface Mechanism for the Chiral-Induced Spin Selectivity Effect: A Critical Perspective.

The chirality-induced spin selectivity (CISS) effect, whereby chiral molecules preferentially transmit electrons of one spin orientation, remains one of the most intriguing and debated phenomena at the interface of spintronics, molecular electronics, and quantum materials. Despite extensive experimental observations across diverse platforms─including transport junctions, photoemission, and enantioselective chemistry─a comprehensive theoretical framework is still lacking. In this perspective, we critically examine the spinterface mechanism as a unifying explanation for the CISS effect. The spinterface model, which hypothesizes a feedback interaction between electron motion in chiral molecules and fluctuating surface magnetic moments, is shown to quantitatively reproduce experimental data across various systems and conditions. We contrast it with some existing theoretical models, highlighting key experimental features. Importantly, we also address open questions and criticisms of this model, including the nature of surface magnetism, the role of dissipation, and the applicability of the mechanism to nonhelical or electrode-free systems. By offering falsifiable predictions and reconciling theory with experimental raw data, this work aims to sharpen the dialogue surrounding the microscopic origin of CISS and stimulate further experimental and theoretical progress.