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Abstract
Strongly correlated materials with multiple order parameters provide unique insights into the fundamental interactions in condensed matter systems and present opportunities for innovative technological applications. A class of antiferromagnetic honeycomb lattices compounds, A
4
B
2
O
9
(A = Co, Fe, Mn; B = Nb, Ta), have been explored owing to the occurrence of linear magnetoelectricity. From our investigation of magnetoelectricity on single crystalline Co
4
Ta
2
O
9
, we discovered strongly nonlinear and antisymmetric magnetoelectric behavior above the spin-flop transition for magnetic fields applied along two orthogonal in-plane directions. This observation suggests that two types of inequivalent Co
2+
sublattices generate magnetic-field-dependent ferroelectric polarization with opposite signs. The results motivate fundamental and applied research on the intriguing magnetoelectric characteristics of these buckled-honeycomb lattice materials.