“…[ 9,10 ] Among others, dimeric clusters of plasmonic NPs show strong optical near‐field coupling and form hotspots in which the electromagnetic field is concentrated, depending on the interparticle distance, the orientation of NPs, and the size, shape and composition of NPs. [ 11–13 ] These unique properties have enabled enormous applications of plasmonic NP dimers in surface enhanced Raman spectroscopy (SERS) detection, [ 14,15 ] mask‐free ultrahigh resolution lithography, [ 16 ] enhanced chemical synthesis, [ 17 ] and nanopixel displays, [ 18 ] to name just a few. Existing strategies for assembling plasmonic NPs into dimers include electrostatic interaction‐regulated assembly, [ 19 ] assembly of site‐specifically functionalized NPs, [ 20,21 ] DNA origami‐templated assembly, [ 22,23 ] and stoichiometric reaction controlled NP bonding.…”