Tunable Magnetic Transition to a Singlet Ground State in a 2D van der Waals Layered Trimerized Kagomé Magnet

Incorporating magnetism into two-dimensional (2D) van der Waals (vdW) heterostructures is crucial for the development of functional electronic and magnetic devices. Here, we show that Nb₃X₈ (X = Cl, Br) is a family of 2D layered trimerized kagomé magnets that are paramagnetic at high temperatures and undergo a first-order phase transition on cooling to a singlet magnetic state. X-ray diffraction shows that a rearrangement of the vdW stacking accompanies the magnetic transition, with high- and low-temperature phases consistent with scanning transmission electron microscopy images of the end members α-Nb₃Cl₈ and β-Nb₃Br₈. The temperature of this transition is systematically varied across the solid solution Nb₃Cl_8-Br (x = 0-8), with x = 6 having transitions near room temperature. The solid solution also varies the optical properties, which are further modulated by the phase transition. As such, they provide a platform on which to understand and exploit the interplay between dimensionality, magnetism, and optoelectronic behavior in vdW materials.