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The observation of spin-dependent transmission of electrons through chiral molecules has led to the discovery of chiral-induced spin selectivity (CISS). The remarkably high efficiency of the spin polarizing effect has recently gained substantial interest due to the high potential for future sustainable hybrid chiral molecule magnetic applications. However, the fundamental mechanisms underlying the chiral-induced phenomena remain to be understood fully. In this work, we explore the impact of chirality on spin angular momentum in hybrid metal/chiral molecule thin-film heterostructures. For this, we inject a pure spin current via spin pumping and investigate the spin-to-charge conversion at the hybrid chiral interface. Notably, we observe a chiral-induced unidirectionality in the conversion. Furthermore, angle-dependent measurements reveal that the spin selectivity is maximum when the spin angular momentum is aligned with the molecular chiral axis. Our findings validate the central role of spin angular momentum for the CISS effect, paving the path toward three-dimensional functionalization of hybrid molecule-metal devices via chirality.

Homochirality is a hallmark of life on Earth. To achieve and maintain homochirality within a prebiotic network, the presence of an environmental factor acting as a chiral agent and providing a persistent chiral bias to prebiotic chemistry is highly advantageous. Magnetized surfaces are prebiotically plausible chiral agents due to the chiral-induced spin selectivity (CISS) effect, and they were utilized to attain homochiral ribose-aminooxazoline (RAO), an RNA precursor. However, natural magnetic minerals are typically weakly magnetized, necessitating mechanisms to enhance their magnetization for their use as effective chiral agents. Here, we report the magnetization of magnetic surfaces by crystallizing enantiopure RAO, whereby chiral molecules induce a uniform surface magnetization due to the CISS effect, which spreads across the magnetic surface akin to an avalanche. Chirality-induced avalanche magnetization enables a feedback between chiral molecules and magnetic surfaces, which can amplify a weak magnetization and allow for highly efficient spin-selective processes on magnetic minerals., (© 2023. Springer Nature Limited.)