Electronic structure, magnetic interactions, and magnonics of 2D trichloride materials

Abstract

Using advanced density functional theory, this study demonstrates the robust thermodynamic, structural, and dynamical stability of pristine, 3d-doped (Ti, Cr), and 4f-doped (Ce) transition metal trichlorides (MCl3). While standard generalized gradient approximation (GGA) incorrectly predicts metallic behavior, hybrid functional calculations successfully capture their semiconducting nature, yielding accurate band gaps of 2.54 eV (VCl3), 4.01 eV (CrCl3), and 2.61 eV (TiCl3). These materials exhibit intrinsic ferromagnetism, with CrCl3 displaying overlapping topological features in both its magnon and phonon dispersions along the high-symmetry K direction, which induces magnon-phonon coupling. Incorporating 3d dopants into VCl3 successfully tunes the bandgap (1.32 eV for Ti and 2.74 eV for Cr) without destroying ferromagnetism, while 4f Ce-doping in CrCl3 introduces localized states below the Fermi level that yield strong nearest-neighbor exchange coupling. Ultimately, this electronic and magnetic tunability highlights the potential of these 2D trichlorides in advanced spintronic functionalities.