Search for: All records

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. 

Abstract High-density phase change memory (PCM) storage is proposed for materials with multiple intermediate resistance states, which have been observed in 1T-TaS₂due to charge density wave (CDW) phase transitions. However, the metastability responsible for this behavior makes the presence of multistate switching unpredictable in TaS₂devices. Here, we demonstrate the fabrication of nanothick verti-lateralH-TaS₂/1T-TaS₂heterostructures in which the number of endotaxial metallicH-TaS₂monolayers dictates the number of resistance transitions in 1T-TaS₂lamellae near room temperature. Further, we also observe optically active heterochirality in the CDW superlattice structure, which is modulated in concert with the resistivity steps, and we show how strain engineering can be used to nucleate these polytype conversions. This work positions the principle of endotaxial heterostructures as a promising conceptual framework for reliable, non-volatile, and multi-level switching of structure, chirality, and resistance.