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Here, we report a highly sensitive and reliable surface enhanced Raman scattering (SERS)-based immunoassay using bimetallic alloy Ag@Au hollow dual-rim nanorings (DRNs) where two hollow nanorings with different diameters are concentrically overlapped and connected by thin metal ligaments, forming circular hot-zones in the intra-nanogaps between the inner and outer rims. Pt DRNs were first prepared, and then Ag was deposited on the surface of the Pt skeleton, followed by Au coating, resulting in alloy Ag@Au hollow DRNs. The chemical stability of Au and the high optical properties of Ag are incorporated into a single entity, Ag@Au hollow DRNs, enabling strong single-particle SERS activity and biocompatibility through surface modification with thiol-containing functionalities. When Ag@Au hollow DRNs were utilized as nanoprobes for detecting human chorionic gonadotropin (HCG) hormone through a SERS-based immunoassay, a very low limit of detection of 10 pM with high reliability was achieved, strongly indicating their advantage as ultrasensitive SERS nanoprobes.

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 paper, we demonstrate the synthesis of morphologically complex nanoframes wherein a mixture of frames and thin solid planes, which we refer to as walled-nanoframes, are present in a single particle. By applying multiple chemical steps including shape evolution of Au nanocrystals and controlling chemical potential of solution for selective deposition, we successfully designed a variety of Pt nanoframes including Pt cuboctahedral nanoframes and Pt single-walled nanoframes. The rationale for on-demand chemical steps with well-faceted Au overgrowth allowed for the synthesis of double-walled nanoframes where two Pt single-walled nanoframes are concentrically overlapped in a single entity with a clearly discernible gap between the two nanoframes. Given the coexistence of an open structure of nanoframe and thin plates within one entity, the double-walled nanoframes showed a dramatic increase in catalytic activity toward the methanol oxidation reaction, acting as high-surface area, carbon-free, and volume-compact nanocatalysts.