Giant exchange splitting in the electronic structure of A-type 2D antiferromagnet CrSBr

In the field of 2D magnetic semiconductors, CrSBr has been the focus of research due to its intriguing magnetic, transport and optical properties that have potential to underpin novel devices. Here we present the evolution of the electronic structure of CrSBr from its antiferromagnetic ground state to the paramagnetic phase. The ground state photoemission data, obtained using a novel method to overcome sample charging issues, is very well reproduced by 𝐐𝐒𝐆Ŵ calculations, a self-consistent many-body perturbative approach that computes electronic eigenfunctions in presence of excitonic correlations. The electronic structure is complex at Γ, but simplifies at the X points of the Brillouin zone where the non-symmorphic lattice symmetry enforces band degeneracies. In the vicinity of these X points, in the deeper-lying valence bands one can identify pairs of states with mainly Br- and S- character. The energy splitting between them is understood as an exchange splitting within the individual layers in which the spins all align, despite the absence of a net magnetic moment in the so-called A-type antiferromagnetic arrangement. By tracing band positions as a function of temperature, we identify that this exchange splitting disappears above T_N, alongside a significant increase in the spectral broadening in all states.