Double-Pulse Femtosecond Laser Fabrication of Highly Ordered Periodic Structures on Au Thin Films Enabling Low-Cost Plasmonic Applications.

Periodic plasmonic arrays, making possible excitations of surface lattice resonances (SLRs) or quasi-resonant features, are of great importance for biosensing and other applications. Fabrication of such arrays over a large area is typically very costly and time-consuming when performed using conventional electron beam lithography and other methods, which reduce application prospects. Here, we propose a technique of double femtosecond pulse (∼170 fs) laser-assisted structuring of thin (∼32 nm) Au films deposited on a glass substrate and report a single-step fabrication of homogeneous and highly ordered Au-based laser-induced periodic surface structures (LIPSS) over a large area. Our experimental results unveil the key importance of the interpulse delay as the determining factor rendering possible the homogeneity of laser-induced structures and confirm that highly ordered, functional LIPSS occurs solely upon double pulse irradiation under a specific interpulse delay range. A theoretical investigation complements experimental results, providing significant insights into the structure formation mechanism. Ellipsometric measurements show that such LIPSS structures can exhibit highly valuable plasmonic features in light reflection. In particular, we observed ultranarrow resonances associated with diffraction-coupled SLRs, which are of paramount importance for biosensing and other applications. The presented data suggest that femtosecond double pulse structuring of thin metal films can serve as a valuable and low-cost tool for large-scale fabrication of highly ordered functional elements and structures.