Giant chirality-induced spin-selectivity of polarons

Abstract: The chirality-induced spin selectivity (CISS) effect gives rise to strongly spin-dependent transport through many organic molecules and structures. Its discovery raises fascinating fundamental questions as well as the prospect of possible applications. The basic phenomenology, a strongly asymmetric magnetoresistance despite the absence of magnetism, is now understood to result from the combination of spin-orbit coupling and chiral geometry. However, experimental signatures of electronic helicity were observed at room temperature, i.e., at an energy scale that exceeds the typical spin-orbit coupling in organic systems by several orders of magnitude. This work shows that a new energy scale for CISS emerges for currents carried by polarons, i.e., in the presence of strong electron-phonon coupling. In particular, we found that polaron fluctuations play a crucial role in the two manifestations of CISS in transport measurements -- the spin-dependent transmission probability through the system and asymmetric magnetoresistance.