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Abstract Superlattice formation dictates the physical properties of many materials, including the nature of the ground state in magnetic materials. Chemical composition is commonly considered to be the primary determinant of superlattice identity, especially in intercalation compounds. Nevertheless, in this work, we find that kinetic control of superlattice growth leads to the coexistence of disparate crystallographic domains within a compositionally perfect single crystal. We demonstrate that Cr_1/4TaS₂is a noncollinear antiferromagnet in which scattering between majority and minority superlattice domains engenders complex magnetotransport below the Néel temperature, including an anomalous Hall effect. We characterize the magnetic phases in different domains, image their nanoscale morphology, and propose a mechanism for nucleation and growth using a suite of experimental probes coupled with first-principles calculations and symmetry analysis. These results provide a blueprint for the deliberate engineering of macroscopic transport responses via microscopic tuning of magnetic exchange interactions in superlattice domains. 

Bragg interferometry (BI) is an imaging technique based on four-dimensional scanning transmission electron microscopy (4D-STEM) wherein the intensities of select overlapping Bragg disks are fit or more qualitatively analyzed in the context of simple trigonometric equations to determine local stacking order. In 4D-STEM based approaches, the collection of full diffraction patterns at each real-space position of the scanning probe allows the use of precise virtual apertures much smaller and more variable in shape than those used in conventional dark field imaging such that even buried interfaces marginally twisted from other layers can be targeted. With a coarse-grained form of dark field ptychography, BI uses simple physically derived fitting functions to extract the average structure within the illumination region and is, therefore, viable over large fields of view. BI has shown a particular advantage for selectively investigating the interlayer stacking and associated moiré reconstruction of bilayer interfaces within complex multi-layered structures. This has enabled investigation of reconstruction and substrate effects in bilayers through encapsulating hexagonal boron nitride and of select bilayer interfaces within trilayer stacks. However, the technique can be improved to provide a greater spatial resolution and probe a wider range of twisted structures, for which current limitations on acquisition parameters can lead to large illumination regions and the computationally involved post-processing can fail. Here, we analyze these limitations and the computational processing in greater depth, presenting a few methods for improvement over previous works, discussing potential areas for further expansion, and illustrating the current capabilities of this approach for extracting moiré-scale strain.