Multiferroicity in a Two-Dimensional Non-van der Waals Crystal of AgCr2X4 (X = S or Se).

Two-dimensional (2D) intrinsic multiferroics have long been pursued not only for their potential technological applications but also as model systems for studying emergent quantum phenomena and coupling mechanisms between various order parameters in low-dimensional space. However, the realization of 2D multiferroics is still a challenge. In this paper, we reveal that 2D AgCr2X4 (X = S or Se) crystals, which have been synthesized from the non-van der Waals (non-vdW) AgCrX2 bulk phase, are type I half-metallic/metallic multiferroics in which ferroelectricity and ferromagnetism coexist. The off-centering displacement of the Ag ion introduces out-of-plane polarization, and the magnetism originates from the interactions between Cr atoms. Remarkably, AgCr2Se4 shows topologically nontrivial spin textures, such as Meron pairs and Néel-type skyrmions, under suitable temperatures and magnetic fields. Our findings demonstrate that 2D multiferroics can be achieved from non-vdW materials and in turn open a new avenue for 2D multiferroics.