Internal Structure Tailoring in 3D Nanoplasmonic Metasurface for Surface-Enhanced Raman Spectroscopy

Tunable nanoplasmonic metasurfaces have resulted in many versatile platforms for sensing applications including surface-enhanced Raman scattering (SERS)-based detection. However, to date, their fabrication still faces challenges in uniformity, repeatability, and controllability. Here, a novel large-area and hierarchical nanoplasmonic array with controlled internal structure and tunable plasmonic properties is reported, relying on controllably tailoring the single nanosphere on a uniform double-layered array into a well-defined nanoflower structure. The fabrication involves colloidal self-assembly, lithography, and plasmonic metal coating. First, a uniformly distributed double-layered colloidal array is fabricated via an ethanol-assisted self-assembly technique. Next, with the help of inductively coupled plasma dry etching, the lower layer is transformed to the nanoflower array with well-defined petal shape. Subsequently, a gold film with controlled thickness is deposited onto the nanoflower structured array, resulting in a tunable optical and SERS-active enhancement effect. Furthermore, 3D finite-difference time-domain simulation shows multiple enhancement sites inside the nanoflower array. Such a brand-new 3D structured array has the potential for varied applications, ranging from SERS sensors to light regulation.