Abstract
CrI2 is a van der Waals layered material that exhibits helimagnetism that propagates along ribbon chains. This is determined from neutron time-of-flight diffraction measurements. Below TN=17 K in the orthorhombic structure, a screwlike helimagnetic order develops with an incommensurate wave vector of q≈(0.2492,0,0) at 8 K. Using density functional theory (DFT)+U calculations, the J1−J2 model is leveraged to describe the helimagnetism, where J1(>0) and J2(<0) correspond, respectively, to a ferromagnetic nearest-neighbor and antiferromagnetic next-nearest-neighbor intrachain interaction. The DFT+U calculations suggest that orthorhombic CrI2 satisfies conditions that favor formation of helimagnetic order.