Large-scale fabrication of highly ordered sub-20 nm noble metal nanoparticles on silica substrates without metallic adhesion layers

Periodic noble metal nanoparticles offer a wide spectrum of applications including chemical and biological sensors, optical devices, and model catalysts due to their extraordinary properties. For sensing purposes and catalytic studies, substrates made of glass or fused-silica are normally required as supports, without the use of metallic adhesion layers. However, precise patterning of such uniform arrays of silica-supported noble metal nanoparticles, especially at sub-100 nm in diameter, is challenging without adhesion layers. In this paper, we report a robust method to large-scale fabricate highly ordered sub-20 nm noble metal nanoparticles, i.e., gold and platinum, supported on silica substrates without adhesion layers, combining displacement Talbot lithography (DTL) with dry-etching techniques. Periodic photoresist nanocolumns at diameters of ~110 nm are patterned on metal-coated oxidized silicon wafers using DTL, and subsequently transferred at a 1:1 ratio into anti-reflection layer coating (BARC) nanocolumns with the formation of nano-sharp tips, using nitrogen plasma etching. These BARC nanocolumns are then used as a mask for etching the deposited metal layer using inclined argon ion-beam etching. We find that increasing the etching time results in cone-shaped silica features with metal nanoparticles on the tips at diameters ranging from 100 nm to sub-30 nm, over large areas of 3×3 cm(2). Moreover, subsequent annealing these sub-30 nm metal nanoparticle arrays at high-temperature results in sub-20 nm metal nanoparticle arrays with ~10(10) uniform particles.