Realizing Square-Ordered Nanopillars with a 0.1-Tera-Density through a Superimposed Masking Strategy for Advanced Surface-Enhanced Raman Spectroscopy

Despite widespread interest in nanoscale pillar structures for various optical devices, including solar cells, photonic crystal lasers, and sensors, the critical challenges for mass production are the high equipment costs and limited scalability of traditional manufacturing methods. To overcome these hurdles, this study develops a simple and highly scalable etch-mask superposition technique based on thermally assisted nanotransfer printing (T-nTP) of Cr line patterns. The orthogonal superposition of linear Cr mask patterns creates double-height cross-point arrays that effectively and selectively protect the underlying SiO₂ during subsequent reactive ion etching. This process generates highly uniform nanoscale pillar arrays with an extremely high density of 0.1 tera-pillars per square inch, eliminating the need for high-cost patterning platforms. As an exemplary application, we demonstrate the use of these perfectly ordered nanopillar arrays as high-performance surface-enhanced Raman scattering (SERS) sensors through the deposition of noble metal films on the nanopillar surface. These nanopillars enable exceptionally uniform SERS intensity with spot variations of less than 7% in methylene blue (MB) measurements. Additionally, they exhibit sensitive detections and accurate quantification for thiabendazole (TBZ) at concentrations as low as 10^-8 M, along with multicycle reusability without noticeable degradation, owing to the outstanding robustness of the SiO₂ nanopillars.