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Register a new userCharting the Exciton-Polariton Landscape in WSe2 Thin Flakes by Cathodoluminescence Spectroscopy
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Semiconducting transition-metal dichalcogenides (TMDCs) provide a fascinating discovery platform for strong light-matter interaction effects in the visible spectrum at ambient conditions. While most of the work has focused on hybridizing excitons with resonant photonic modes of external mirrors, cavities, or nanostructures, intriguingly, TMDC flakes of sub-wavelength thickness can themselves act as nanocavities. Here, we determine the optical response of such freestanding planar waveguides of WSe$_2$, by means of cathodoluminescence spectroscopy. We reveal strong exciton-photon interaction effects that foster long-range propagating exciton-polaritons and enable direct imaging of the energy transfer dynamics originating from cavity-like Fabry-Perot resonances. Furthermore, confinement effects due to discontinuities in the flakes are demonstrated as an efficient means to tailor the exciton-photon coupling strength, along the edges of natural flakes. Our combined experimental and theoretical results provide a deeper understanding of exciton-photon self-hybridization in semiconducting TMDCs and may pave the way to optoelectronic nanocircuits exploiting exciton-photon interaction.
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Polaritons enable the resonant coupling of excitons and photons to vibrations in the application-relevant super high frequency (SHF, 3-30 GHz) domain. We introduce a novel platform for coherent optomechanics based on the coupling of exciton-polaritons and electrically driven SHF longitudinal acoustic phonons confined within the spacer region of a planar Bragg microcavity. An intrinsic property of the microcavity platform is the back-feeding of phonons via reflections at the sample boundaries, which enables frequency x quality factors products exceeding 10^14 Hz as well as huge modulation amplitudes of the optical transition energies (up to 8 meV). We show that the modulation is dominated by the phonon-induced energy shifts of the excitonic polariton component, thus leading to an oscillatory transition between the regimes of weak and strong light-matter coupling. These results open the way for polariton-based coherent optomechanics in the non-adiabatic, side-band-resolved regime of coherent control.
Exciton-polaritons in semiconductor microcavities have advanced to become a model system for studying dynamical Bose-Einstein condensation, macroscopic coherence, many-body effects, nonclassical states of light and matter, and possibly quantum phase transitions in a solid state. Being low mass bosons, these light-matter quasiparticles can condense at comparably high temperatures up to 300K, while preserving fundamental properties such as coherence in space and time domain even when they are out of equilibrium with the environment. Although the presence of an in-plane polariton confinement potential is not strictly necessary in order to observe condensation of polaritons, engineering the polariton confinement is a key to controlling, shaping and directing the flow of polaritons. Prototype polariton-based optoelectronic devices rely on ultrafast photon-like velocities and strong nonlinearities, as well as on tailored confinement. Nanotechnology provides several pathways to achieving such a confinement, and the specific features and advantages of the different techniques are discussed in this paper. As hybrid exciton-photon quasiparticles, polaritons can be trapped via their excitonic as well as their photonic component, which leads to a wide choice of highly complementary techniques. Here we highlight the almost free choice of trapping geometries and depths of confinement that provides a powerful tool for control and manipulation of polariton systems both in semi-classical and quantum domain. Furthermore, the possibility to observe effects of polariton blockade, Mott insulator physics, and population of higher-order bands in sophisticated lattice potentials is discussed. The observation of such effects will signify the opportunity for the realization of novel polaritonic non-classical light sources and quantum simulators.
Polaritons formed by the coupling of light and material excitations such as plasmons, phonons, or excitons enable light-matter interactions at the nanoscale beyond what is currently possible with conventional optics. Recently, significant interest has been attracted by polaritons in van der Waals materials, which could lead to applications in sensing, integrated photonic circuits and detectors. However, novel techniques are required to control the propagation of polaritons at the nanoscale and to implement the first practical devices. Here we report the experimental realization of polariton refractive and meta-optics in the mid-infrared by exploiting the properties of low-loss phonon polaritons in isotopically pure hexagonal boron nitride (hBN), which allow it to interact with the surrounding dielectric environment comprising the low-loss phase change material, Ge$_3$Sb$_2$Te$_6$ (GST). We demonstrate waveguides which confine polaritons in a 1D geometry, and refractive optical elements such as lenses and prisms for phonon polaritons in hBN, which we characterize using scanning near field optical microscopy. Furthermore, we demonstrate metalenses, which allow for polariton wavefront engineering and sub-wavelength focusing. Our method, due to its sub-diffraction and planar nature, will enable the realization of programmable miniaturized integrated optoelectronic devices, and will lay the foundation for on-demand biosensors.
Bogoliubovs theory states that self-interaction effects in Bose-Einstein condensates produce a characteristic linear dispersion at low momenta. One of the curious features of Bogoliubovs theory is that the new quasiparticles in the system are linear combinations of creation and destruction operators of the bosons. In exciton-polariton condensates, this gives the possibility of directly observing the negative branch of the Bogoliubov dispersion in the photoluminescence (PL) emission. Here we theoretically examine the PL spectra of exciton-polariton condensates taking into account of reservoir effects. At sufficiently high excitation densities, the negative dispersion becomes visible. We also discuss the possibility for relaxation oscillations to occur under conditions of strong reservoir coupling. This is found to give a secondary mechanism for making the negative branch visible.
We experimentally demonstrate hot exciton transport in h-BN encapsulated WSe2 monolayers via spatially and temporally resolved photoluminescence measurements at room temperature. We show that the nonlinear evolution of the mean squared displacement of the non-resonantly excited hot exciton gas is primarily due to the relaxation of its excess kinetic energy and is characterized by a density-dependent fast expansion that converges to a slower, constant rate expansion. We also observe saturation of the hot exciton gas expansion rate at high excitation densities due to the balance between Auger-assisted hot exciton generation and the phonon-assisted hot exciton relaxation processes.
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