Twisted oxide membrane interface by local atomic registry design

Interplay of lattice, orbital, and charge degrees of freedom in complex oxide materials has hosted a plethora of exotic quantum phases and physical properties. Recent advances in synthesis of freestanding complex oxide membranes and twisted heterostructures assembled from membranes provide new opportunities for discovery using moiré design with local lattice control. To this end, we designed moiré crystals at the coincidence site lattice condition, providing commensurate structure within the moiré supercell arising from the multi-atom complex oxide unit cell. We fabricated such twisted bilayers from freestanding SrTiO3 membranes and used depth sectioning-based TEM methods to discover ordered charge states at the moiré interface. By selectively imaging SrTiO3 atomic planes at different depths through the bilayer, we clearly resolved the moiré periodic structure at the twisted interface and found that it exhibits lattice-dependent charge disproportionation in the local atomic registry within the moiré supercell. Our density-functional modelling of the twisted oxide interface predicts that these moiré phenomena are accompanied by the emergence of a two-dimensional flat band that can drive new electronic phases. Our work provides a novel guideline for controlling moiré periodicity in twisted oxides and opens pathways to exploit the new functionalities via moiré lattice-driven charge-orbital correlation.