First-principles study and mesoscopic modeling of two-dimensional spin and orbital fluctuations in FeSe

Abstract

We calculated the structural, electronic, and magnetic properties of FeSe within density-functional theory at the generalized gradient approximation level. First, we studied how the bandwidth of the d-bands at the Fermi energy is renormalized by adding simple corrections: Hubbard U, Hund's J, and by introducing long-range magnetic orders. We found that introducing either a striped or a staggered dimer antiferromagnetic order brings the bandwidths—which are starkly overestimated at the generalized gradient approximation level—closer to those experimentally observed. Second, for the ferromagnetic, the striped, checkerboard, and staggered dimer antiferromagnetic order, we investigate the change in magnetic formation energy with local magnetic moment of Fe at a pressure up to 6 GPa. The bilinear and biquadratic exchange energies are derived from the Heisenberg model and noncollinear first-principles calculations, respectively. We found a nontrivial behavior of the spin-exchange parameters on the magnetization, and we put forward a field-theory model that rationalizes these results in terms of two-dimensional spin and orbital fluctuations. The character of these fluctuations can be either that of a standard density wave or a topological vortex. Topological vortices can result in mesoscopic magnetization structures. Published by the American Physical Society 2024