Interplay of Structural Chirality, Electron Spin and Topological Orbital in Chiral Molecular Spin Valves

Chirality has been a property of central importance in chemistry and biology for more than a century, and is now taking on increasing relevance in condensed matter physics. Recently, electrons were found to become spin polarized after transmitting through chiral molecules, crystals, and their hybrids. This phenomenon, called chirality-induced spin selectivity (CISS), presents broad application potentials and far-reaching fundamental implications involving intricate interplays among structural chirality, topological states, and electronic spin and orbitals. However, the microscopic picture of how chiral geometry influences electronic spin remains elusive. In this work, via a direct comparison of magnetoconductance (MC) measurements on magnetic semiconductor-based chiral molecular spin valves with normal metal electrodes of contrasting strengths of spin-orbit coupling (SOC), we unambiguously identified the origin of the SOC, a necessity for the CISS effect, given the negligible SOC in organic molecules. The experiments revealed that a heavy-metal electrode provides SOC to convert the orbital polarization induced by the chiral molecular structure to spin polarization. Our results evidence the essential role of SOC in the metal electrode for engendering the CISS spin valve effect. A tunneling model with a magnetochiral modulation of the potential barrier is shown to quantitatively account for the unusual transport behavior. This work hence produces critical new insights on the microscopic mechanism of CISS, and more broadly, reveals a fundamental relation between structure chirality, electron spin, and orbital.