Optical Introduction and Manipulation of Plasmon-Exciton-Trion Coupling in a Si/WS2/Au Nanocavity.

Strong plasmon-exciton coupling, which has potential applications in nanophotonics, plasmonics, and quantum electrodynamics, has been successfully demonstrated by using metallic nanocavities and two-dimensional materials. Dynamical control of plasmon-exciton coupling strength, especially by using optical methods, remains a big challenge although it is highly desirable. Here, we report the optical introduction and manipulation of plasmon-exciton-trion coupling realized in a dielectric-metal hybrid nanocavity, which is composed of a silicon (Si) nanoparticle and a thin gold (Au) film, with an embedded tungsten disulfide (WS2) monolayer. We employ scattering and photoluminescence spectra to characterize the coupling strength between plasmons and excitons in Si/WS2/Au nanocavities constructed by using Si nanoparticles with different diameters. We enhance the plasmon-exciton and plasmon-trion coupling strength by injecting excitons and trions into the WS2 monolayer with a 488 nm laser beam. It is revealed that the emission intensities of excitons and trions with respect to the reference WS2 monolayer can be modified through the change in the coupling strength induced by the laser light. Interestingly, the coupling strength between the plasmons and the excitons/trions can be manipulated from weak to strong coupling regime by simply increasing the laser power, which is clearly resolved in the scattering spectra of Si/WS2/Au nanocavities. More importantly, the plasmon-exciton-trion coupling induced by the laser light is confirmed by the energy exchange between excitons and trions. Our findings indicate the possibility for optically manipulating plasmon-exciton interaction and suggest the practical applications of dielectric-metal hybrid nanocavities in nanoscale plasmonic devices.

Greatly Enhanced Plasmon-Exciton Coupling in Si/WS2/Au Nanocavities.

A strong light-matter interaction is highly desirable from the viewpoint of both fundamental research and practical application. Here, we propose a dielectric-metal hybrid nanocavity composed of a silicon (Si) nanoparticle and a thin gold (Au) film and investigate numerically and experimentally the coupling between the plasmons supported by the nanocavity and the excitons in an embedded tungsten disulfide (WS2) monolayer. When a Si/WS2/Au nanocavity is excited by the surface plasmon polariton generated on the surface of the Au film, greatly enhanced plasmon-exciton coupling originating from the hybridization of the surface plasmon polariton, the mirror-image-induced magnetic dipole, and the exciton modes is clearly revealed in the angle- or size-resolved scattering spectra. A Rabi splitting as large as ∼240 meV is extracted by fitting the experimental data with a coupled harmonic oscillator model containing three oscillators. Our findings open new horizons for constructing nanoscale photonic devices by exploiting dielectric-metal hybrid nanocavities.

Radiation of the high-order plasmonic modes of large gold nanospheres excited by surface plasmon polaritons.

Large metallic nanoparticles with sizes comparable to the wavelength of light are expected to support high-order plasmon modes exhibiting resonances in the visible to near infrared spectral range. However, the radiation behavior of high-order plasmon modes, including scattering spectra and radiation patterns, remains unexplored. Here, we report on the first observation and characterization of the high-order plasmon modes excited in large gold nanospheres by using the surface plasmon polaritons generated on the surface of a thin gold film. The polarization-dependent scattering spectra were measured by inserting a polarization analyzer in the collection channel and the physical origins of the scattering peaks observed in the scattering spectra were clearly identified. More interestingly, the radiation of electric quadrupoles and octupoles was resolved in both frequency and spatial domains. In addition, the angular dependences of the radiation intensity for all plasmon modes were extracted by fitting the polarization-dependent scattering spectra with multiple Lorentz line shapes. A significant enhancement of the electric field was found in the gap plasmon modes and it was employed to generate hot-electron intraband luminescence. Our findings pave the way for exploiting the high-order plasmon modes of large metallic nanoparticles in the manipulation of light radiation and light-matter interaction.

High Q-factor with the excitation of anapole modes in dielectric split nanodisk arrays.

The simultaneous realization of high Q-factor resonances and strong near-field enhancements around and inside of dielectric nanostructures is important for many applications in nanophotonics. However, the incident fields are often confined within dielectric nanoparticles, which results in poor optical interactions with external environment. Near-field enhancements can be extended outside of dielectric nanostructures with proper design, but the Q-factor is often reduced caused by additional radiation losses. This paper shows that the obstacles to achieve high Q-factor, that is, the radiative losses can be effectively suppressed by using dielectric nanodisk arrays, where the Q-factor is about one order larger than that of the single disks associated with the nonradiating anapole modes and the collective oscillations of the arrays. When the resonance energies of the electric dipole mode and the subradiant mode are degenerate with each other, the destructive interference produces an effect analogous to electromagnetically induced transparency. Furthermore, the Q-factor can be extremely enlarged with dielectric split nanodisk arrays, where the present of the split gap does not induce additional losses. Instead, the coupling between the two interfering modes is modified by adjusting the gap width, which makes it possible to achieve high Q-factor and strong near-field enhancements around and inside of the split disks simultaneously. It is shown that the Q-factor is approaching to 106 when the gap width is about 110 nm, and the near-field enhancements around and inside of the split disks are about two orders stronger than that of the single disk.

Anticrossing double Fano resonances generated in metallic/dielectric hybrid nanostructures using nonradiative anapole modes for enhanced nonlinear optical effects.

Third-harmonic generation with metallic or dielectric nanoparticles often suffer from, respectively, small modal volumes and weak near-field enhancements. This study propose and demonstrate that a metallic/dielectric hybrid nanostructure composed of a silver double rectangular nanoring and a silicon square nanoplate can be used to overcome these obstacles for enhanced third-harmonic generation. It is shown that the nonradiative anapole mode of the Si plate can be used as a localized source to excite the dark subradiant octupole mode of the Ag ring, and the mode hybridization leads to the formation of an antibonding and a bonding subradiant collective mode, thereby forming anticrossing double Fano resonances. With the strong coupling between individual particles and the effectively suppressed radiative losses of the Fano resonances, several strong hot spots are generated around the Ag ring due to the excitation of the octupole mode, and electromagnetic fields within the Si plate are also strongly amplified, making it possible to confine more incident energy inside the dielectric nanoparticle. Calculation results reveal that the confined energy inside the Si plate and the Ag ring for the hybrid structures can be about, respectively, more than three times and four orders stronger than that of the corresponding isolated nanoparticles, which makes the designed hybrid nanostructure a promising platform for enhanced third-harmonic generation.