Spin polarization driven by molecular vibrations leads to enantioselectivity in chiral molecules

Chirality pervades multiple scientific domains-physics, chemistry, biology, and astronomy-and profoundly influences their foundational principles. Recently, the chirality-induced spin selectivity (CISS) phenomenon has captured significant attention in physical chemistry due to its potential applications and intriguing underlying physics. Despite its prominence, the microscopic mechanisms of CISS remain hotly debated, hindering practical applications and further theoretical advancements. Here we challenge the established view that attributes CISS-related phenomena to current-induced spin polarization and electron transport across interfaces. We propose that molecular vibrations in chiral molecules primarily drive spin polarization, thereby governing CISS. Employing an electrochemical cell paired with a precisely engineered magnetic multilayer, we demonstrate that the magnetic interactions akin to interlayer exchange coupling are crucial for CISS. Our theoretical study suggests that molecular vibrations facilitate chirality-dependent spin polarization, which plays a pivotal role in CISS-related phenomena such as magnetoresistance and enantiomer separation using ferromagnets. These findings necessitate a paradigm shift in the design and analysis of systems in various scientific fields, extending the role of spin dynamics from traditional areas such as solid-state physics to chemical reactions, molecular biology, and even drug discovery.