Light-Induced Spin Slanting in 2D Multiferroic Magnet

Controlling the spin orientation of two-dimensional (2D) materials has emerged as a frontier of condensed-matter physics, resulting in the discovery of various phases of matter. However, in most cases, spin orientation can be established only at specific directions of out-of-plane and in-plane, which is a drawback compared with three-dimensional systems, limiting exploration of novel physics. Here, we introduce a methodology for manipulating spin slanting in 2D multiferroic materials through ultrafast pulses of light. Based on model analysis, we find that simultaneous triggering of spin–orbit coupling-induced interactions from in-plane and out-of-plane orbitals can generate spin slanting. By choosing 2D multiferroic materials with specific low-energy composition endowed by symmetry, such triggering can be readily achieved through ultrafast light illumination, leading to light-induced spin slanting. Using real-time time-dependent density-functional theory, we demonstrate this approach in multiferroic single-layer CuCr 2 Se 4 . This study provides an efficient way to manipulate spin orientation in 2D materials and establishes a general platform to explore the physics and applications associated with spin slanting.