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Two-dimensional (2D) plasmonic nanoassemblies are programmable ultrathin materials that one can, in principle, adjust the size and shape of their constituent building blocks to fine-tune collective optical, electrical, and mechanical properties. Here, we report a new 2D nanoassembly from structurally complex plasmonic building blocks, namely, matryoshka-like gold (Au) nanoframes. Using a seed-mediated alternating deposition of Au and silver (Ag) elements in conjunction with a selective etching process, we obtain monodisperse matryoshka-like Au nanoframes with a nesting number (Nn) of up to 5. A cubic nanoframe displays dominant intraplasmonic coupling attributed to bonding and antibonding dipolar modes, which shift to blue and red, respectively, with an increased Nn. Combined with polystyrene (PS) ligand exchange and drying-mediated self-assembly, the approach mentioned above can be used to produce 2D plasmonic matryoshka nanoassemblies. Both experimental and simulation results demonstrate the presence of intra- and inter-ridge plasmonic coupling in the nanoassemblies. The 5-nested nanomatryoshka assemblies exhibit a Raman enhancement 14-fold greater than those with 1-nested cubic nanomatryoshka, demonstrating the dominant intraridge hot spot effects. Taking advantage of interparticle distance-dependent optical transparency of 2D matryoshka nanoframe assemblies, we further demonstrate temperature-enabled encryption/decryption using thermoresponsive polymers.
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