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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. 

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.