Cracking enabled unclonability in colloidal crystal patterns authenticated with computer vision

. A serious issue accompanying the facile chemical self-assembly approach to colloidal crystals is the formation of uncontrolled and irregular cracks. In contrast to the previous efforts to avoid cracking, the unfavorable and random micro-cracks in colloidal crystals were utilized here as unclonable codes for tamper-proof anti-counterfeiting. The special structural and optical characteristics of the colloidal crystal patterns assembled with monodisperse poly(styrene-methyl methacrylate-acrylic acid) core-shell nanospheres enabled multi-anti-counterfeiting modes, including angle-dependent structural colors and polarization anisotropy, besides the physically unclonable functions (PUFs) of random micro-cracks. Moreover, by using the random cracks in the colloidal crystals as templates to guide fluorescent silica nanoparticle deposition, an fluorescent anti-counterfeiting mode with PUFs was introduced. To validate the PUFs of the fluorescent micro-cracks in the colloidal crystals, a novel edge-sensitive template matching approach based on a computer vision algorithm with an accuracy of ∼100% was developed, enabling ultimate security immune to forgery. The computer-vision verifiable physically unclonable colloidal crystals with multi-anti-counterfeiting modes are superior to conventional photonic crystal anti-counterfeiting materials that rely on angle-dependent or tunable structural colors, and the conventional PUF labels in the aspect of decorative functions, which will open a new avenue for advanced security materials with multi-functionality.