Mind the Gap - Imaging Buried Interfaces in Twisted Oxide Moirés

Abstract: The ability to tune electronic structure in twisted stacks of layered, two-dimensional (2D) materials has motivated the exploration of similar moir\'e physics with stacks of twisted oxide membranes. Due to the intrinsic three-dimensional (3D) nature of bonding in many oxides, achieving atomic-level coupling is significantly more challenging than in 2D van der Waals materials. Although clean interfaces with atomic level proximity have been demonstrated in ceramic bicrystals using high-temperature and high-pressure processing to facilitate atomic diffusion that flattens rough interfaces, such conditions are not readily accessible when bonding oxide membranes. This study shows how topographic mismatch due to surface roughness of the membranes can restrict atomic-scale proximity at the interface to isolated patches even after obvious issues of contaminants and amorphous interlayers are eliminated. In hybrid interfaces between a chemically inert 2D material and an oxide membrane, the reduced ability of the 2D material to conform to the membrane's step-terrace topography also limits atomic-scale contact. In all these material systems, the interface morphology is best characterized using cross-sectional imaging and is necessary to corroborate investigations of interlayer coupling. When imaging the bicrystal in projection, conventional through-focal imaging is found to be relatively insensitive to the buried interface, whereas electron ptychography reliably resolves structural variations on the order of a nanometer. These findings highlight interface roughness as a key challenge for the field of oxide twistronics and emphasizes the need for reliable characterization methods.