Controlling orbital ordering of intergrowth structures with flat [Ag(II)F2] layers to mimic oxocuprates(II)

Based on the Density Functional Theory calculations, we propose a new pathway toward compounds featuring flat [AgF2] layers which mimic [CuO2] layers in high-temperature oxocuprate superconductor precursors. Calculations predict the dynamic (phonon) and energetic stability of the new phases over diverse substrates. For some compounds with ferro orbital ordering, we find a gigantic intrasheet superexchange constant of up to –211 meV (DFT+U) and –256 meV (SCAN), calculated for hypothetical (CsMgF3)2KAgF3 intergrowth. Semiempirical calculations show that at optimum doping, the expected superconducting critical temperature should reach 200 K. The partial substitution of K+ with Ba2+ leads to noticeable electron doping of [AgF2] sublattice, as revealed by progressive population of the Upper-Hubbard band. On the other hand, modest 10-15% hole-doping through partial substitution of Mg2+ with Li+, primarily leads to the depopulation of p(z) orbitals of apical F atoms. We also find structures with an undesired antiferrodistortive structural ordering and discuss the structural factors that determine the transition from buckled to flat planes and from different types of orbital ordering using Landau theory of phase transitions.The database consists of structure calculated within DFT+U framework.