One‐Dimensional Magnetic MX₃ Single‐Chains (M = Cr, V and X = Cl, Br, I)

Abstract Magnetic materials in reduced dimensions are not only excellent platforms for fundamental studies of magnetism, but they play crucial roles in technological advances. The discovery of intrinsic magnetism in monolayer 2D van der Waals systems has sparked enormous interest, but the single‐chain limit of 1D magnetic van der Waals materials has been largely unexplored. This paper reports on a family of 1D magnetic van der Waals materials with composition MX 3 (M = Cr, V, and X = Cl, Br, I), prepared in fully‐isolated fashion within the protective cores of carbon nanotubes. Atomic‐resolution scanning transmission electron microscopy identifies unique structures that differ from the well‐known 2D honeycomb lattice MX 3 structure. Density functional theory calculations reveal charge‐driven reversible magnetic phase transitions.