Controlling plasmonic systems with nanometre resolution in transparent films and their colors over large non-planar areas is a key issue for spreading their use in various industrial fields. Using light to direct self-organization mechanisms provides high-speed and flexible processes to meet this challenge. Here, we describe a route for the laser-induced self-organization of metallic nanostructures in 3D. Going beyond the production of planar nanopatterns, we demonstrate that ultrafast laser-induced excitation combined with non-linear feedback mechanisms in a nanocomposite thin film can lead to 3D self-organized nanostructured films. The process, which can be extended to complex layered composite systems, produces highly uniform large-area nanopatterns. We show that 3D self-organization originates from the simultaneous excitation of independent optical modes at different depths in the film and is activated by the plasmon-induced charge separation and thermally-induced NP growth mechanisms. This laser color marking technique enables multiplexed optical image encoding and the generated nanostructured Ag NPs:TiO 2 films offer great promise for applications in solar energy harvesting, photocatalysis or photochromic devices.
KeywordsUltrafast photonics; Laser-induced self-organization; Nanostructured thin film; plasmonic nanomaterials; plasmonic colors Controlling metallic nanostructures over large non-planar areas with high flexibility and speed is of strategic importance for developing industrial applications of plasmonic systems.