Quasi‐1D van der Waals Antiferromagnetic CrZr4Te14 with Large In‐Plane Anisotropic Negative Magnetoresistance

The discovery of 2D van der Waals (vdW) magnetic materials is of great significance to explore intriguing 2D magnetic physics and develop innovative spintronic devices. In this work, a new quasi‐1D vdW layered compound CrZr4Te14 is successfully synthesized. Owing to the existence of 1D [CrTe2] and [ZrTe3] chains along the b‐axis, CrZr4Te14 crystals show strong anisotropy of phonon vibrations, electrical transport, and magnetism. Density functional theory calculations reveal the ferromagnetic (FM) coupling within the [CrTe2] chain, while the interchain and interlayer couplings are both weakly antiferromagnetic (AF). Notably, a large intrinsic negative magnetoresistance (nMR) of −56% is achieved at 2 K under 9 T, and the in‐plane anisotropic factor of nMR can reach up to 8.2 in the CrZr4Te14 device. The 1D FM chains and anisotropic nMR effect make CrZr4Te14 an interesting platform for exploring novel polarization‐sensitive spintronics. Layered CrZr4Te14 is constructed of [CrTe2] and [ZrTe3] chains along the b‐axis. The intrachain magnetic coupling of the [CrTe2] chain is ferromagnetic, while the opposite magnetic ordering between the chains makes CrZr4Te14 an antiferromagnet. Moreover, CrZr4Te14 shows large intrinsic negative magnetoresistence of −56%, and the in‐plane anisotropic factor reaches 8.2 owing to the ferromagnetic [CrTe2] chains.