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In this article, we make our effort to scale up the synthesis of gold nanorods (GNRs) using the modified strategy. The prepared GNRs are self-assembled vertically to the substrate over an large micrometer-size area without external fields. We also demonstrate that this complex superstructure is an excellent surface-enhanced Raman scattering (SERS) substrate with uniform electric field enhancement, high intensity of hot spots and reproducible enhancement factors (EFs) in the desirable spectral range. For practical perspective, the substrate shows great promise for fluorescence and luminescence.

Large-area and Free-standing 3D Superlattices Induced by Droplet Evaporation