“…Of particular interest is the creation of uniformly narrow gaps, with precise control of gap size on noble metal substrates, ideally using low-cost, high-yield, and time-saving techniques. Various nanofabrication methods, such as electron-beam/extreme-ultraviolet lithography (EBL/EUV) [ 13 , 14 , 15 ], focused-ion beam (FIB) milling [ 16 , 17 , 18 ], metal nanoparticles assembly [ 19 , 20 , 21 ], nanosphere lithography (NSL) [ 22 , 23 , 24 ], capillary force-assisted lithography [ 25 , 26 ], block copolymer lithography (BCL) [ 27 , 28 ], interference lithography [ 29 , 30 , 31 ], and DNA origami [ 32 , 33 , 34 , 35 ] have been developed and used to pattern highly hierarchical ordered metallic nanostructures with nanogap features for the purpose of making SERS substrates. Among these methods, for instance, EBL/EUV methods are still not stable and reproducible enough to create nanogaps down to 10 nm, which are well known for obtaining ultra-strong electromagnetic field enhancement [ 12 , 36 ], and, additionally, are cost-intensive and time-consuming for fabricating nanostructures over wide areas.…”