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Register a new userStrong Interaction of Cherenkov Radiation with Excitons in WSe2 Crystals
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The optical responses of semiconducting transition metal dichalcogenides are dominated by excitons. Being able to strongly interact with light and other materials excitations, excitons in semiconductors are prototypes for investigating many-particle and strong-field physics, including exciton-exciton, exciton-photon, and exciton-phonon interactions. Strong exciton-photon interactions, in particular, can lead to the emergence of exciton-polariton hybrid quasiparticles with peculiar characteristics, and a tendency toward macroscopic and spontaneous coherence. Normally, far-field and near-field optical spectroscopy techniques are used to investigate exciton-photon interactions. Here, we demonstrate that the radiation generated by moving electrons in transition metal dichalcogenides, namely Cherenkov radiation, can strongly interact with excitons. We investigate the coherence properties and spectral signatures of exciton-photon interactions in TMDC bulk crystals, using cathodoluminescence spectroscopy. Our findings lay the ground for cathodoluminescence spectroscopy and in particular electron-beam techniques as probes of exciton-polariton spontaneous coherence in semiconductors, beyond the well-known plasmonic investigations.
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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.
We theoretically analyse the hybrid Mie-exciton optical modes arising from the strong coupling of excitons in organic dyes or transition-metal dichalcogenides with the Mie resonances of high-index dielectric nanoparticles. Detailed analytic calculations show that silicon--exciton core--shell nanoparticles are characterised by a richness of optical modes which can be tuned through nanoparticle dimensions to produce large anticrossings in the visible or near infrared, comparable to those obtained in plexcitonics. The complex magnetic-excitonic nature of these modes is understood through spectral decomposition into Mie-coefficient contributions, complemented by electric and magnetic near-field profiles. In the frequency range of interest, absorptive losses in silicon are sufficiently low to allow observation of several periods of Rabi oscillations in strongly coupled emitter-particle architectures, as confirmed here by discontinuous Galerkin time-domain calculations for the electromagnetic field beat patterns. These results suggest that Mie resonances in high-index dielectrics are promising alternatives for plasmons in strong-coupling applications in nanophotonics, while the coupling of magnetic and electric modes opens intriguing possibilities for external control.
The strong light-matter coupling of a microcavity mode to tightly bound Frenkel excitons in organic materials emerged as a versatile, room-temperature compatible platform to study nonlinear many-particle physics and bosonic condensation. However, various aspects of the optical response of Frenkel excitons in this regime remained largely unexplored. Here, we utilize a hemispheric optical cavity filled with the fluorescent protein mCherry to address two important questions in the field of room-temperature polariton condensates. First, combining the high quality factor of the microcavity with a well-defined mode structure allows us to provide a definite answer whether temporal coherence in such systems can become competitive with their low-temperature counterparts. We observe highly monochromatic and coherent light beams emitted from the condensate, characterized by a coherence time greater than 150$,$ps, which exceeds the polariton lifetime by two orders of magnitude. Second, the high quality of our device allows to sensibly trace the emission energy of the condensate, and thus to establish a fundamental picture which quantitatively explains the core nonlinear processes yielding the characteristic density-dependent blueshift. We find that the energy shift of Frenkel exciton-polaritons is largely dominated by the reduction of the Rabi-splitting due to phase space filling effects, which is influenced by the redistribution of polaritons in the system. While our finding of highly coherent condensation at ambient conditions addresses the suitability of organic polaritonics regarding their utilization as highly coherent room temperature polariton lasers, shedding light on the non-linearity is of great benefit towards implementing non-linear devices, optical switches, and lattices based on exciton-polaritons at room temperature.
Spatially indirect excitons with displaced wavefunctions of electrons and holes play a pivotal role in a large portfolio of fascinating physical phenomena and emerging optoelectronic applications, such as valleytronics, exciton spin Hall effect, excitonic integrated circuit and high-temperature superfluidity. Here, we uncover three types of spatially indirect excitons (including their phonon replicas) and their quantum-confined Stark effects in hexagonal boron nitride encapsulated bilayer WSe2, by performing electric field-tunable photoluminescence measurements. Because of different out-of-plane electric dipole moments, the energy order between the three types of spatially indirect excitons can be switched by a vertical electric field. Remarkably, we demonstrate, assisted by first-principles calculations, that the observed spatially indirect excitons in bilayer WSe2 are also momentum-indirect, involving electrons and holes from Q and K/{Gamma} valleys in the Brillouin zone, respectively. This is in contrast to the previously reported spatially indirect excitons with electrons and holes localized in the same valley. Furthermore, we find that the spatially indirect intervalley excitons in bilayer WSe2 can exhibit considerable, doping-sensitive circular polarization. The spatially indirect excitons with momentum-dark nature and highly tunable circular polarization open new avenues for exotic valley physics and technological innovations in photonics and optoelectronics.
Moire superlattices provide a powerful tool to engineer novel quantum phenomena in two-dimensional (2D) heterostructures, where the interactions between the atomically thin layers qualitatively change the electronic band structure of the superlattice. For example, mini-Dirac points, tunable Mott insulator states, and the Hofstadter butterfly can emerge in different types of graphene/boron nitride moire superlattices, while correlated insulating states and superconductivity have been reported in twisted bilayer graphene moire superlattices. In addition to their dramatic effects on the single particle states, moire superlattices were recently predicted to host novel excited states, such as moire exciton bands. Here we report the first observation of moire superlattice exciton states in nearly aligned WSe2/WS2 heterostructures. These moire exciton states manifest as multiple emergent peaks around the original WSe2 A exciton resonance in the absorption spectra, and they exhibit gate dependences that are distinctly different from that of the A exciton in WSe2 monolayers and in large-twist-angle WSe2/WS2 heterostructures. The observed phenomena can be described by a theoretical model where the periodic moire potential is much stronger than the exciton kinetic energy and creates multiple flat exciton minibands. The moire exciton bands provide an attractive platform to explore and control novel excited state of matter, such as topological excitons and a correlated exciton Hubbard model, in transition metal dichalcogenides.
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