The interplay between chirality and magnetism is a source of fascination among scientists for over a century. In recent years, chirality-induced spin selectivity (CISS) has attracted renewed interest. It is observed that electron transport through layers of homochiral molecules leads to a significant spin polarization of several tens of percent. Despite the abundant experimental evidence gathered through mesoscopic transport measurements, the exact mechanism behind CISS remains elusive. This study reports spin-selective electron transport through single helical aromatic hydrocarbons that are sublimed in vacuo onto ferromagnetic cobalt surfaces and examined with spin-polarized scanning tunneling microscopy (SP-STM) at a temperature of 5 K. Direct comparison of two enantiomers under otherwise identical conditions revealed magnetochiral conductance asymmetries of up to 50% when either the molecular handedness is exchanged or the magnetization direction of the STM tip or Co substrate is reversed. Importantly, the results rule out electron-phonon coupling and ensemble effects as primary mechanisms responsible for CISS.

Fakultät für Physik Universität Duisburg Essen 47057 Duisburg Germany

Institut für Chemie Universität Zürich 8057 Zürich Switzerland

Jülich Aachen Research Alliance Fundamentals of Future Information Technology Forschungszentrum Jülich 52425 Jülich Germany

Molecular Surface Science Group Empa Swiss Federal Laboratories for Materials Science and Technology 8600 Dübendorf Switzerland

Nanosurf Laboratory Institute of Physics The Czech Academy of Sciences 16200 Prague Czech Republic

Peter Grünberg Institute Electronic Properties Forschungszentrum Jülich 52425 Jülich Germany

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An aperiodic chiral tiling by topological molecular self-assembly