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With the discovery of two-dimensional (2D) ferroelectricity and ferromagnetism in van der Waals (vdW) materials, there has been significant interest in 2D multiferroics. Herein, we report the occurrence of weak ferromagnetism and magnetoelectricity in vdW antiferromagnet MnPSe3 single crystals. Our results demonstrate that MnPSe3 undergoes an antiferromagnetic transition at the Néel temperature TN = 70 K with weak ferromagnetism along the [1–10] direction. Detailed magnetoelectric (ME) data show that MnPSe3 exhibits a linear ME tensor αij with nine nonzero components. Additionally, a magnetically induced electric polarization as large as 98.5 μC/m2 is observed along the [110] direction, with a ME coefficient of 13.5 ps/m at 10 K for a magnetic field of 9 T applied along the [110] direction. Importantly, we discuss our experiments based on symmetry and microscopic analysis, thereby suggesting that the spin-dependent p-d hybridization mechanism plays an important role in the emergence of magnetic-field-induced ferroelectricity. Hence, our findings provide insights for exploring the ME coupling in vdW materials. [ABSTRACT FROM AUTHOR]

With the discovery of two-dimensional (2D) ferroelectricity and ferromagnetism in van der Waals (vdW) materials, there has been significant interest in 2D multiferroics. Herein, we report the occurrence of weak ferromagnetism and magnetoelectricity in vdW antiferromagnet MnPSe3 single crystals. Our results demonstrate that MnPSe3 undergoes an antiferromagnetic transition at the Néel temperature TN = 70 K with weak ferromagnetism along the [1–10] direction. Detailed magnetoelectric (ME) data show that MnPSe3 exhibits a linear ME tensor αij with nine nonzero components. Additionally, a magnetically induced electric polarization as large as 98.5 μC/m2 is observed along the [110] direction, with a ME coefficient of 13.5 ps/m at 10 K for a magnetic field of 9 T applied along the [110] direction. Importantly, we discuss our experiments based on symmetry and microscopic analysis, thereby suggesting that the spin-dependent p-d hybridization mechanism plays an important role in the emergence of magnetic-field-induced ferroelectricity. Hence, our findings provide insights for exploring the ME coupling in vdW materials. [ABSTRACT FROM AUTHOR]