Unexpected large nanoparticle size of single dimer hotspot systems for broadband SERS enhancement.

We have numerically demonstrated the feasibility and possibility to achieve broadband surface-enhanced Raman scattering (SERS) enhancement in the visible and near-infrared wavelength range using single nanoparticle (NP) dimer hotspot systems. Instead of the conventionally reported sub-100 nm, we find that the optimal NP size is as large as 200 nm in diameter for both Ag and Au. The key lies in the continuous arising of the bonding dipole plasmon mode and higher-order resonances at shorter wavelengths. Further, it is revealed that the near- and far-field optical responses of these hotspot systems correlate well with each other, despite the intrinsic enormous near- to far-field redshift for individual large NPs. The physical principles demonstrated here benefit significantly the fundamental understanding and engineering optimization of broadband SERS substrates.