Mind the Gap -- Imaging Buried Interfaces in Twisted Oxide Moirés

Abstract

The ability to tune electronic structure in twisted stacks of two-dimensional (2D) materials has motivated the exploration of similar moiré physics with twisted oxide membranes. Due to the intrinsic three-dimensional nature of bonding in many oxides, achieving atomic-level coupling is significantly more challenging than with 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 contaminants and amorphous interlayers are eliminated. In interfaces between 2D materials and oxide membranes the reduced ability of the 2D material to conform to the membrane's step-terrace topography also limits atomic-scale contact. When imaging stacked membranes in projection, we find conventional through-focal imaging to be relatively insensitive to the buried interface, whereas electron ptychography detects structural variations on the order of a nanometer. These findings highlight interface roughness as a key challenge for the field of oxide twistronics and emphasize the need for reliable characterization methods, both in cross-section and projection.

40 pages, 7 figures, 20 supplementary figures