PHYSICAL REVIEW B 100, 045116 (2019) Linear-response description of superexchange-driven orbital ordering in K2CuF4

We study the nature of orbital and magnetic order in the layered perovskite K2CuF4, and compare to the case of the infinite-layer system KCuF3. To this end, we augment the local-density approximation + dynamical mean-field theory technique with linear-response functions. We explain orbital and magnetic order, and their evolution with increasing pressure. We show that both the tetragonal (εT) and the Jahn-Teller (εJT) crystal-field splitting play a key role. We find that surprisingly, unlike in KCuF3, εT is comparable to, or even larger than, εJT; in addition, εT is mostly determined by the layered structure itself and by the compression of the K cage, rather than by the deformations of the CuF6 octahedra. Next, we study the nature of orbital order. We calculate the superexchange transition temperature, finding TKK ∼ 300 K, a value close to the one for KCuF3. Thus, in K2CuF4 as in KCuF3, TKK is too small to explain the existence of orbital order up to the melting temperature. We show, however, that in the case of the layered perovskite, an additional superexchange mechanism is at work. It is an orbital Zeeman term, ĥKK , and it is active also above TKK . We show that due to ĥKK , phases with different types of ordering can coexist at temperatures below TKK . Similar effects are likely to play a role in other layered correlated systems.