Laser‐Scanning‐Guided Assembly of Quasi‐3D Patterned Arrays of Plasmonic Dimers for Information Encryption

Abstract The application of plasmonic dimeric nanostructures in color displays, data storage, and especially metamaterials necessitates the patterning of dimers into ordered arrays, but controllable assembly of plasmonic nanoparticles into patterned dimer arrays on substrates still remains a challenge. Here, a facile laser‐scanning‐based strategy to fabricate quasi‐3D patterned arrays of plasmonic nanoparticle dimers with controlled orientation for plasmonic information encryption is reported. Laser scanning of polymer‐covered plasmonic nanoparticle (e.g., gold) arrays selectively exposes the surface of irradiated nanoparticle via localized photothermal heating, guiding the assembly of another type of nanoparticles onto the exposure nanoparticle surface to form dimers on substrates. This combined top‐down/bottom‐up approach is highly flexible in forming high‐resolution patterns of plasmonic dimers from nanoparticles of different sizes and shapes. The z ‐axis orientation, interparticle spacing, and nanoparticle size and shape of plasmonic dimers can be precisely tuned, enabling the modulation of the coupled resonances of the dimer arrays. Moreover, it is demonstrated that the patterned dimer arrays can be used in information encryption where their plasmonic color can be repeatedly displayed and erased. This work provides an important addition to tools for the fabrication of patterned complex plasmonic nanostructures from as‐synthesized nanoparticles with broad applications.