Strained Epitaxy of Monolayer Transition Metal Dichalcogenides for Wrinkle Arrays

Wrinkling two-dimensional (2D) transition metal dichalcogenides (TMDCs) provides a mechanism to adjust the physical and chemical properties as per need. Traditionally, TMDCs wrinkles achieved by transferring exfoliated materials on prestretched polymer suffer from poor control and limited sample area, which significantly hinders desirable applications. Herein, we fabricate large-area monolayer TMDCs wrinkle arrays directly on the m-quartz substrate using strained epitaxy. The uniaxial thermal expansion coefficient mismatch between the substrate and TMDCs materials enables the generation of large uniaxial thermal strain. By quenching the TMDCs after growth, this uniaxial thermal strain can be quickly released as a form of wrinkle arrays along the [0001]_quartz direction. Using WS₂ as a model system, the size of as-grown wrinkles can be finely modulated within sub-100 nm by changing the quenching temperature. These WS₂ wrinkles can be locally folded and form various multilayer structures with odd layer numbers during the transfer process. Besides, the corrugated structures in WS₂ wrinkles induce significant changes to optical properties including anisotropic Raman response, enhanced photoluminescence, and second harmonic generation emissions. Furthermore, these wrinkle arrays exhibit enhanced chemical reactivity that can be selectively engineered to ribbon arrays with improved electrocatalytic performance. The developed strategy of strained epitaxy here should enable flexibility in the design of more sophisticated 2D-based structures, offering a simple but effective way toward the modulation of properties with enhanced performances.