“…Distinct from their bulk counterparts or disordered clusters, emergent properties, and corresponding structure–function relationships of such well-defined superlattices are elucidated, such as the coherent vibrational modes, plasmon propagation, unique mechanical properties, , metal–insulator transition, p -type conductivities, and plasmon-driven catalytic properties, etc. By taking advantage of the strong coupling of metal nanoparticles with light at specific photon energies, enhanced light-matter interaction and electromagnetic field can be generated across the superlattices, which inspiring broad range of promising applications, including SERS based sensing and imaging, ,− flexible optoelectronics, energy harvest systems . However, it has proven to be remarkably difficult to build high-quality superlattices with macroscopic scale while maintaining nanoscopic ordering due to the complex interparticle forces during self-assembly …”