Electronic excitations and spin interactions in chromium trihalides from embedded many-body wavefunctions.

ABSTRACT: Although chromium trihalides are widely regarded as a promising class of two-dimensional magnets for next-generation devices, an accurate description of their electronic structure and magnetic interactions has proven challenging to achieve. Here, we quantify electronic excitations and spin interactions in CrX ₃ (X = Cl, Br, I) using embedded many-body wavefunction calculations and fully generalized spin Hamiltonians. We find that the three trihalides feature comparable d-shell excitations, consisting of a high-spin ⁴ A ₂ (t2g3eg0) ground state lying 1.5-1.7 eV below the first excited state ⁴ T ₂ ( t2g2eg1 ). CrCl₃ exhibits a single-ion anisotropy A _sia = - 0.02 meV, while

SUBMITTER: Yadav R 

PROVIDER: S-EPMC11364507 | biostudies-literature | 2024

REPOSITORIES: biostudies-literature