Figure 1.

(a) Tetragonal 2×2×2 supercell (32 formula units) employed to model Mn:CsPbCl₃. Orange, Mn; purple, Cl; cyan, Pb; and blue, Cs atoms. (b) Qualitative molecular orbital scheme for the complex with spin (↑) (blue) and spin (↓) (red) manifolds. (c) Total (gray) and manganese (blue) density of states (DOS) of ⁶Mn²⁺:CsPbCl₃ computed at the PBE0 and PBE0-SOC levels (solid and dashed lines, respectively), with Mn molecular orbitals labeled. (d) Aligned manganese DOS for the ⁶MnCl₆^4– model complex. (e) Isodensity plots of representative ⁶Mn²⁺:CsPbCl₃ spin α single-particle states with e_g, t_2g, t_2g*, and e_g* character.