Electronic structure and magnetic ordering of the semiconducting chromium trihalides CrCl3, CrBr3, and CrI3

We present results from an electronic structure investigation of the chromium halides CrCl(3), CrBr(3), and CrI(3), as obtained by the linearized augmented plane wave method of density functional theory. Our interest focuses on the chloride. While all three halides display strong ferromagnetic coupling within the halide-Cr-halide triple layers, our emphasis is on differences in the interlayer magnetic coupling. In agreement with experimental results, our calculations indicate ferromagnetic ordering for CrBr(3) as well as CrI(3). The antiferromagnetic state of CrCl(3) can be reproduced by introducing an on-site electron-electron repulsion. However, we observe that the ground state depends critically on the specific approach used. Our results show that a low temperature structural phase transition from monoclinic to trigonal is energetically favourable for CrCl(3).