Orbital Longitudinal Magneto-electric Coupling in Multilayer Graphene

Magneto-electric coupling enables the manipulation of magnetization by electric fields and vice versa. While typically found in heavy element materials with large spin-orbit coupling, recent experiments on rhombohedral-stacked pentalayer graphene (RPG) have demonstrated a { longitudinal magneto-electric coupling} (LMC) without spin-orbit coupling. Here we present a microscopic theory of LMC in multilayer graphene and identify how it is controlled by a ``layer-space'' quantum geometry and interaction-driven valley polarization. Strikingly, we find that the interplay between valley-polarized order and LMC produces a butterfly shaped magnetic hysteresis controlled by out-of-plane electric field: a signature of LMC and a multiferroic valley order. Furthermore, we identify a nonlinear LMC in multilayer graphene under time-reversal symmetry, while the absence of centrosymmetry enables the generation of a second-order nonlinear electric dipole moment in response to an out-of-plane magnetic field. Our theoretical framework provides a quantitative understanding of LMC, as well as the emergent magneto-electric properties of multilayer graphene.