Low-Dimensional Magnetic Semimetal Cr0.65Al1.35Se3.

While exploring novel magnetic semiconductors, the new phase Cr0.65Al1.35Se3 was discovered and characterized by both structural and physical properties. Cr0.65Al1.35Se3 was found to crystallize into orthorhombic CrGeTe3-type structure with space group Pnma (no. 62). Vacancies and mixed occupancies were tested, and the results show that one of the 4c sites accommodates a mixture of Cr and Al atoms, while the other 4c site is fully occupied by Al atoms. Unique structural features include a T-shaped channel network created from the edge-sharing Cr/Al@Se6 and Al@Se4 polyhedra and a zipper effect of the puckered Se atoms inside the columnar channels. The round peak observed in the temperature-dependent magnetic susceptibility (χg) plot at ∼8(1) K corresponds to the antiferromagnetic-type transition in Cr0.65Al1.35Se3. However, the positive θCW indicates an additional ferromagnetic interaction, which is highly likely due to the complex magnetic structure arising from the mixed Cr/Al occupancies on the 4c site. Electrical resistivity measurements confirm that Cr0.65Al1.35Se3 is a semimetal with a positive magnetoresistance. Here we present the characterization and determination of the crystal structure and physical properties for this new material.