Anisotropic metallic heterotrimer systems for an ultrahigh plasmonic-based improvement of hyper-Raman scattering signal

Abstract

Abstract An anisotropic metallic trimer is proposed as an active plasmonic substrate for an ultrahigh enhancement in the spectroscopic signal of the hyper-Raman scattering (HRS) process. The suggested three-particle system is composed from non-aligned asymmetric nanoparticles of a cubic shape. The interacting resonators are made of gold material and illuminated by a longitudinally polarized light. The non-alignment condition in the heterotrimer is achieved by shifting the intermediate cube transversely away from the interparticle axis. Optical cross-section, nearfield distribution and charge density are calculated by using the finite-difference time-domain electrodynamic simulation tool. The enhancement factor of the HRS is calculated theoretically from the nearfield intensity associated with the resonance phenomenon of the considered trimer. The extinction profile of the illuminated system exhibits the excitation of two plasmonic modes. A superradiant mode observed in the longer wavelength region which resulted from the in-phase coupling between the plasmonic modes excited in each one of the three resonators. The second mode is a subradiant band emerged from the interference between bright and dark modes. The resonance wavelength of these two modes matches the excitation one and the second-order Stockes condition, respectively. After optimizing the value of both the transverse shift and the gap spacing, the enhancement factor of the HRS can reach as high as a value never reported before of 1 × 1018.