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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. 

Abstract The construction of thin film heterostructures has been a widely successful archetype for fabricating materials with emergent physical properties. This strategy is of particular importance for the design of multilayer magnetic architectures in which direct interfacial spin-spin interactions between magnetic phases in dissimilar layers lead to emergent and controllable magnetic behavior. However, crystallographic incommensurability and atomic-scale interfacial disorder can severely limit the types of materials amenable to this strategy, as well as the performance of these systems. Here, we demonstrate a method for synthesizing heterostructures comprising magnetic intercalation compounds of transition metal dichalcogenides (TMDs), through directed topotactic reaction of the TMD with a metal oxide. The mechanism of the intercalation reaction enables thermally initiated intercalation of the TMD from lithographically patterned oxide films, giving access to a family of multi-component magnetic architectures through the combination of deterministic van der Waals assembly and directed intercalation chemistry. 

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. 

1T–TaS2 is a layered charge density wave (CDW) crystal exhibiting sharp phase transitions and associated resistance changes. These resistance steps could be exploited for information storage, underscoring the importance of controlling and tuning the CDW states. Given the importance of out-of-plane interactions in 1T–TaS2, modulating interlayer interactions by heterostructuring is a promising method for tailoring CDW phase transitions. In this work, we investigate the optical and electronic properties of heterostructures comprising 1T–TaS2 and monolayer 1H–WSe2. By systematically varying the thickness of 1T–TaS2 and its azimuthal alignment with 1H–WSe2, we find that intrinsic moiré strain and interfacial charge transfer introduce CDW disorder in 1T–TaS2 and modify the CDW ordering temperature. Furthermore, our studies reveal that the interlayer alignment impacts the exciton dynamics in 1H–WSe2, indicating that heterostructuring can concurrently tailor the electronic phases in 1T–TaS2 and the optical properties of 1H–WSe2. This work presents a promising approach for engineering the optoelectronic behavior of heterostructures that integrate CDW materials and semiconductors. 

In conventional ferroelectric materials, polarization is an intrinsic property limited by bulk crystallographic structure and symmetry. Recently, it has been demonstrated that polar order can also be accessed using inherently non-polar van der Waals materials through layer-by-layer assembly into heterostructures, wherein interfacial interactions can generate spontaneous, switchable polarization. Here, we show that deliberate interlayer rotations in multilayer vdW heterostructures modulate both the spatial ordering and switching dy- namics of polar domains. The engendered tunability is unparalleled in conventional bulk ferroelectrics or polar bilayers. By means of operando transmission electron microscopy we show how alterations of the relative rotations of three WSe2 layers produce structural poly- types with distinct arrangements of polar domains with either a global or localized switching response. Furthermore, the presence of uniaxial strain generates structural anisotropy that yields a range of switching behaviors, coercivities, and even tunable biased responses. We also provide evidence of mechanical coupling between the two interfaces of the trilayer, a key consideration for the control of switching dynamics in polar multilayer structures more broadly. 

Moiré superlattices formed by twisting trilayers of graphene are a useful model for studying correlated electron behaviour and offer several advantages over their formative bilayer analogues, including a more diverse collection of correlated phases and more robust superconductivity. Spontaneous structural relaxation alters the behaviour of moiré superlattices considerably and has been suggested to play an important role in the relative stability of superconductivity in trilayers. Here we use an interferometric four-dimensional scanning transmission electron microscopy approach to directly probe the local graphene layer alignment over a wide range of trilayer graphene structures. Our results inform a thorough understanding of how reconstruction modulates the local lattice symmetries crucial for establishing correlated phases in twisted graphene trilayers, evincing a relaxed structure that is markedly different from that proposed previously.