Electric-field control of two-dimensional ferromagnetic properties by chiral ionic gating

Abstract: Chiral molecular systems offer unique pathways to control spin and magnetism beyond conventional symmetry operations. Here, we demonstrate that chiral ionic liquids enable electric-field modulation of two-dimensional (2D) ferromagnetism in FeSi(111) thin films via electric double-layer transistor (EDLT) gating. FeSi hosts chemically-stable, surface-confined ferromagnetism without bulk moments, making the interfacial spins highly responsive to chiral-ion adsorption. Using both achiral and chiral ionic liquids, we systematically compare electrochemical and electrostatic gating effects. While both gating modes modulate magnetic properties such as anomalous Hall conductivity and coercive field, only chiral ionic gating biases the ratio of up- and down-magnetized domains in a handedness-dependent manner, evidencing chirality-induced symmetry breaking. This work establishes chiral ion gating as a novel strategy for controlling magnetic order and opens new directions for chiral spintronics.