Emergent surface magnetic ordering and surface electronic dipole layers in a two-dimensional spin=1/2 La2CuO4 film

The surfaces of strongly correlated materials can exhibit exotic properties that differ substantially from the bulk. Investigation of these surface effects requires both high quality surfaces, and an experimental technique capable of disentangling surface and underneath layers or bulk. Herein, we overcome these two challenges, using newly developed grazing-incident-angle resonant soft x-ray and magnetic scattering techniques to study ultrathin films of Spin(S) = 1/2 La₂CuO₄, the parent compound of high-critical-temperature (high-Tc) superconductor. We observe emergent surface magnetic ordering and surface-like electronic dipole layers at room temperature. As a function of temperature, intrinsic holes from Cu²⁺ and O²⁻ ions are mitigated from the surface into subsurface layers and back into the surface. The intrinsic hole and oxygen ion mitigation have different rates, yielding strong temperature hysteresis. Supported with theoretical calculations, these surface orderings consist of a mixture of Cu²⁺ 3d⁹ (S = 1/2) and Cu¹⁺ 3d¹⁰-like (S = 0) with strong magneto-electronic coupling through the many-body upper Hubbard band. Our results highlight intrinsic holes and oxygen ion mitigations, yielding surface-like electronic dipole and magnetic orderings and the potential of grazing-incident-angle resonant soft X-ray and magnetic scattering to elucidate, layer-by-layer, magnetic and electronic structures."