An engineered CARS substrate with giant field enhancement in crisscross dimer nanostructure.

We theoretically investigate the optical properties of a nanostructure consisting of the two identical and symmetrically arranged crisscrosses. A plasmonic Fano resonance is induced by a strong interplay between bright mode and dark modes, where the bright mode is due to electric dipole resonance while dark modes originate from the magnetic dipole induced by LC resonances. In this article, we find that the electric field "hotspots" corresponding to three different wavelengths can be positioned at the same spatial position, and its spectral tunability is achieved by changing geometric parameters. The crisscrosses system can be designed as a plasmonic substrate for enhancing Coherent Anti-Stokes Raman Scattering (CARS) signal. This discovery provides a new method to achieve single molecule detection. At the same time, it also has many important applications for multi-photon imaging and other nonlinear optical processes, such as four-wave mixing and stimulated Raman scattering.