Strong coupling between plasmons and excitons in nanocavities can result in the formation of hybrid plexcitonic states. Understanding the dispersion relation of plexcitons is important both for fundamental quantum science and for applications including optoelectronics and nonlinear optics devices. The conventional approach, based on statistics over different nanocavities, suffers from large inhomogeneities from the samples, owing to the nonuniformity of nanocavities and the lack of control over the locations and orientations of the excitons. Here we report the first measurement of the dispersion relationship of plexcitons in an individual nanocavity. Using a single silver nanorod as a Fabry-Pérot nanocavity, we realize strong coupling of plasmon in single nanocavity with excitons in a single atomic layer of tungsten diselenide. The plexciton dispersion is measured by in situ redshifting the plasmon energy via successive deposition of a dielectric layer. Room-temperature formation of plexcitons with Rabi splittings as large as 49.5 meV is observed. The realization of strong plasmon-exciton coupling by in situ tuning of the plasmon provides a novel route for the manipulation of excitons in semiconductors.
The interaction between plasmons in metal nanostructures and excitons in layered materials attracts recent interests due to its fascinating properties inherited from the two constituents, e.g., the high tunability on its spectral or spatial properties from the plasmonic component, and the large optical nonlinearity or light emitting properties from the excitonic counterpart. Here, we demonstrate light-emitting plexcitons from the coupling between the neutral excitons in monolayer WSe and highly confined nanocavity plasmons in the nanocube-over-mirror system. We observe, simultaneously, an anticrossing dispersion curve of the hybrid system in the dark-field scattering spectrum and a 1700 times enhancement in the photoluminescence. We attribute the large photoluminescence enhancement to the increased local density of states by both the plasmonic and excitonic constituents in the intermediate coupling regime. In addition, increasing the confinement of the hybrid systems is achieved by shrinking down the size of the hot spot within the gap between the nanocube and the metal film. Numerical calculations reproduce the experimental observations and provide the effective number of excitons taking part in the interaction. This highly compact system provides a room temperature testing platform for quantum cavity electromagnetics at the deep subwavelength scale.
Plasmon rulers can be used for resolving ultrasmall environmental, dimensional, and material changes owing to their high sensitivity associated with a light-scattering spectral shift in response to changes in the separation between plasmonic nanostructures. Here, we show, in several experimental setups, how cavity plasmons in a metal nanowire-on-mirror setup can be used to probe vertical dimensional changes with sub-picometer differential resolutions using two carefully chosen material systems. Specifically, we monitor the dielectric layer thickness changes in response to growth using atomic-layer deposition and to thermal expansion, demonstrating a sensitivity of 14-nm spectral shift per Ångström thickness change and 0.58 pm of vertical differential resolution, respectively. The findings confirm theoretical predictions and highlight the potential use of cavity plasmons in some ultrasensitive sensing applications.
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