The
enhanced second-harmonic generation (SHG) from a monolayer WS2 coupled to a plasmonic nanocavity is experimentally and theoretically
investigated. The nanocavity is comprised of monodispersed Ag nanocubes
separated from an Ag film by a spacer Al2O3,
namely, the nanoparticle on mirror (NPoM) system. When the surface
plasmon polariton resonance (SPPR) wavelength of NPoM nanocavity overlaps
well with the SHG wavelength of the monolayer WS2 (namely,
harmonic resonance), a ∼300-fold SHG enhancement is achieved
in experiment. For theoretical understanding, the quantum mechanical
density matrix method has been used to develop a theory for SHG. It
is found that the SHG intensity of nanohybrid is proportional to the
square of the local-field intensity in NPoM nanocavity at SHG wavelength,
which is ascribed to the dipole–quadrupole interaction between
dipole, P
SHG, in the monolayer WS2 and quadrupole, Q
Ag, in Ag nanocavity.
It is significantly different from that in metal nanoparticles under
harmonic resonance, which is proportional to the local-field intensity.
Therefore, it provides a novel mechanism for enhancing SHG signals
from metal–semiconductor nanohybrids, which has potential applications
in nonlinear devices and hybrid nonlinear metasurfaces.