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For years, solution processing has provided a versatile platform to extendthe applications of transition metal dichalcogenides (TMDs) beyond thoseachievable with traditional preparation methods. However, existingsolution-based synthesis and exfoliation approaches are not compatible withcomplex geometries, particularly when interfacial control is desired. As aresult, promising TMD structures, including MoS2/WS2 heterostructures, arebarred from the rich assembly and modification opportunities possible withsolution preparation. Here, we introduce a strategy that combines traditionalvapor phase deposition and solution chemistry to build TMD core-shellheterostructures housed in aqueous media. We report the first synthesized TMDcore-shell heterostructure, Au@MoS2@WS2, with an Au nanoparticle core and MoS2and WS2 shells, and provide a means of suspending the structure in solution toallow for higher order patterning and ligand-based functionalization.High-resolution electron microscopy and Raman spectroscopy provide detailedanalysis of the structure and interfaces of the core-shell heterostructures.UV-vis, dynamic light scattering, and zeta potential measurements exhibit theoutstanding natural stability and monodispersity of Au@MoS2@WS2 in solution. Asa proof of concept, the aqueous environment is utilized to both functionalizethe core-shell heterostructures with electrostatic ligands and pattern theminto desired configurations on a target substrate. This work harnesses theadvantages of vapor phase preparation of nanomaterials and the functionalitypossible with aqueous suspension to expand future engineering and applicationopportunities of TMD heterostructures.

Au@MoS2@WS2 Core-Shell Architectures: A Solution to Versatile Colloidal Suspensions of 2D Heterostructures