Discovery of orbital ordering in Bi₂Sr₂CaCu₂O_8+x

The primordial ingredient of cuprate superconductivity is the CuO₂ unit cell. Theories usually concentrate on the intra-atom Coulombic interactions dominating the 3d⁹ and 3d¹⁰ configurations of each copper ion. However, if Coulombic interactions also occur between electrons of the 2p⁶ orbitals of each planar oxygen atom, spontaneous orbital ordering may split their energy levels. This long-predicted intra-unit-cell symmetry breaking should generate an orbitally ordered phase, for which the charge transfer energy ε separating the 2p⁶ and 3d¹⁰ orbitals is distinct for the two oxygen atoms. Here we introduce sublattice-resolved ε(r) imaging to CuO₂ studies and discover intra-unit-cell rotational symmetry breaking of ε(r). Spatially, this state is arranged in disordered Ising domains of orthogonally oriented orbital order bounded by dopant ions, and within whose domain walls low-energy electronic quadrupolar two-level systems occur. Overall, these data reveal a Q = 0 orbitally ordered state that splits the oxygen energy levels by ~50 meV, in underdoped CuO₂.