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Here we report a synthetic pathway toward Au truncated octahedral dual-rim nanoframes wherein two functional facets are formed including (1) eight hot nanogaps formed by hexagonal nanoframes embracing core circular nanorings for near-field focusing and (2) six flat squares that facilitate the formation of well-ordered arrays of nanoframes through self-assembly. The existence of intra-nanogaps in a single entity enables strong electromagnetic near-field focusing, allowing single-particle surface-enhanced Raman spectroscopy. Then, we built "all-hot-spot bulk SERS substrates" with those entities, wherein the presence of truncated terraces with high homogeneity in size and shape facilitate spontaneous self-assembly into a highly ordered and uniform superlattice, exhibiting a limit of detection of attomolar concentrations toward 2-naphthalenethiol, which is 6 orders lower than that of monorim counterparts. The observed low limit of detection originates from the combined synergic effect from both inter- and intraparticle coupling in a superlattice, which we dubbed "all-hot-spot bulk SERS substrates".

In this Letter, a rational and stepwise method for the solution-phase synthesis of asymmetric Au split nanorings by adopting Au nanoprisms as a template has been demonstrated. The selective chemical etching of Au nanoprism tips activated the surface reactivity of edges and led to the selective deposition of Pt at the periphery of Au nanoplates. By controlling the total amount of Pt on the edges, different degrees of split Au@Pt nanorings were obtained; the subsequent Au coating around the Au@Pt scaffold eventually resulted in asymmetric Au hexagonal split nanorings. Their surface plasmonic features as a function of split degrees were investigated, including straight nanorods, bent nanorods, split nanorings, and full nanorings. The electrical field focusing using single-particle surface-enhanced Raman spectroscopy was evaluated under different polarization angles of the incident light for two different structures with the point gap and line gap between two arms.

Silver double nanorings with circular intra-nanogaps between two nanorings of different diameters were synthesized without a linker molecule to confine an incident electromagnetic field in a single entity. We used on-demand, rational, and systematic multi-stepwise reactions consisting of (1) selective etching of gold, (2) rim-on deposition of platinum, (3) eccentric growth of gold, and (4) concentric growth of silver. The resulting silver double nanorings exhibited a high degree of homogeneity in both shape and size, with strongly coupled circular hot zones (or "hot halos", referring to the circular intra-nanogaps capable of focusing the near electromagnetic field) resulting from strong surface plasmon coupling between the inner and outer nanorings. Remarkably, these silver double nanorings exhibited strong, stable, and reproducible single-particle surface-enhanced Raman scattering signals without blinking. The signals appeared independently of polarization directions, which is a unique feature of a circular hot halo. The estimated enhancement factor was between 2 × 108 and 7 × 108. The measured limit of detection was 10-7 M in bulk concentration, and the signal appeared 570 s after sample exposure.