Signatures of pressure-enhanced helimagnetic order in van der Waals multiferroic NiI$_2$

Abstract: The van der Waals (vdW) type-II multiferroic NiI$_2$ has emerged as a candidate for exploring non-collinear magnetism and magnetoelectric effects in the 2D limit. Frustrated intralayer exchange interactions on a triangular lattice result in a helimagnetic ground state, with spin-induced improper ferroelectricity stabilized by the interlayer interactions. Here we investigate the magnetic and structural phase transitions in bulk NiI$_2$, using high-pressure Raman spectroscopy, optical linear dichroism, and x-ray diffraction. We obtain evidence for a significant pressure enhancement of the antiferromagnetic and helimagnetic transition temperatures, at rates of $\sim15.3/14.4$ K/GPa, respectively. These enhancements are attributed to a cooperative effect of pressure-enhanced interlayer and third-nearest-neighbor intralayer exchange. These results reveal a general path for obtaining high-temperature type-II multiferroicity via high pressures in vdW materials.