Non-classical Temperature Dependence of Chirality-Induced Magnetization and Its Implications for RNA's Homochirality

Abstract: The single-handedness of biomolecules is a characteristic feature of life on Earth, yet achieving and maintaining a homochiral prebiotic network is a significant challenge. In our previous studies, we reached homochirality in an RNA precursor, ribo-aminooxazoline (RAO), using magnetized magnetite surfaces as chiral reagents, due to the chiral-induced spin selectivity (CISS) effect. We further demonstrated that RAO can induce net magnetization on previously demagnetized surfaces, indicating a self-reinforcing feedback between chiral molecules and magnetic surfaces. However, these processes depend on spin interactions that generally weaken at higher temperatures, raising concerns about the robustness of our mechanisms in natural settings. Additionally, the temperature dependence of CISS remains poorly understood. To address these questions, we investigated the temperature dependence of chirality-induced magnetization. Contrary to classical expectations, we observed a significant increase in induced net magnetization with increasing temperatures, suggesting a phonon-assisted process. Concurrently, we noted a corresponding increase in the relative yield of RAO during its prebiotic synthesis. Our results support a vibronic contribution to CISS and indicate that spin-controlled processes leading to RNA homochirality can occur reliably and effectively over a range of temperatures likely present in prebiotic environments.