LAUSR

Subwavelength periodic confinement can collectively and selectively enhance local light intensity and enable control over the photoinduced phase transformations at the nanometer scale. Standard nanofabrication process can result in geometrical and compositional inhomogeneities in optical phase change materials, especially chalcogenides, as those materials exhibit poor chemical and thermal stability. Here the self‐assembled planar chalcogenide nanostructured array is demonstrated with resonance‐enhanced light emission to create an all‐dielectric optical metasurface, by taking advantage of the fluid properties associated with solution‐processed films. A patterned silicon membrane serves as a template for shaping the chalcogenide metasurface structure. Solution‐processed arsenic sulfide metasurface structures are self‐assembled in the suspended 250 nm silicon membrane templates. The periodic nanostructure dramatically manifests the local light–matter interaction such as absorption of incident photons, Raman emission, and photoluminescence. Also, the thermal distribution is modified by the boundaries and thus the photothermal crystallization process, leading to the formation of anisotropic nanoemitters within the field enhancement area. This hybrid structure shows wavelength‐selective anisotropic photoluminescence, which is a characteristic behavior of the collective response of the resonant‐guided modes in a periodic nanostructure. The resonance‐enhanced Purcell effect can manifest the quantum efficiency of localized light emission.