Spatial Tuning of Light–Matter Interaction via Strain-Gradient-Induced Polarization in Freestanding Wrinkled 2D Materials

To date, controlled deformation of two-dimensional (2D) materials has been extensively demonstrated with substrate-supported structures. However, interfacial effects arising from these supporting materials may suppress or alter the unique behavior of the deformed 2D materials. To address interfacial effects, we report, for the first time, the formation of a micrometer-scale freestanding wrinkled structure of 2D material without any encapsulation layers where we observed the enhanced light–matter interactions with a spatial modulation. Freestanding wrinkled monolayer WSe₂ exhibited about a 330% enhancement relative to supported wrinkled WSe₂ quantified through photoinduced force microscopy. Spatial modulation and enhancement of light interaction in the freestanding wrinkled structures are attributed to the enhanced strain-gradient effect (i.e., out-of-plane polarization) enabled by removing the constraining support and proximate dielectrics. Our findings offer an additional degree of freedom to modulate the out-of-plane polarization and enhance the out-of-plane light–matter interaction in 2D materials.