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Register a new userExciton-exciton interaction beyond the hydrogenic picture in a MoSe$_2$ monolayer in the strong light-matter coupling regime
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In transition metal dichalcogenides layers of atomic scale thickness, the electron-hole Coulomb interaction potential is strongly influenced by the sharp discontinuity of the dielectric function across the layer plane. This feature results in peculiar non-hydrogenic excitonic states, in which exciton-mediated optical nonlinearities are predicted to be enhanced as compared to their hydrogenic counterpart. To demonstrate this enhancement, we performed optical transmission spectroscopy of a MoSe$_2$ monolayer placed in the strong coupling regime with the mode of an optical microcavity, and analyzed the results quantitatively with a nonlinear input-output theory. We find an enhancement of both the exciton-exciton interaction and of the excitonic fermionic saturation with respect to realistic values expected in the hydrogenic picture. Such results demonstrate that unconventional excitons in MoSe$_2$ are highly favourable for the implementation of large exciton-mediated optical nonlinearities, potentially working up to room temperature.
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The valley pseudospin in monolayer transition metal dichalcogenides (TMDs) has been proposed as a new way to manipulate information in various optoelectronic devices. This relies on a large valley polarization that remains stable over long timescales (hundreds of ns). However, time resolved measurements report valley lifetimes of only a few ps. This has been attributed to mechanisms such as phonon-mediated inter-valley scattering and a precession of the valley psedospin through electron-hole exchange. Here we use transient spin grating to directly measure the valley depolarization lifetime in monolayer MoSe$_{2}$. We find a fast valley decay rate that scales linearly with the excitation density at different temperatures. This establishes the presence of strong exciton-exciton Coulomb exchange interactions enhancing the valley depolarization. Our work highlights the microscopic processes inhibiting the efficient use of the exciton valley pseudospin in monolayer TMDs.
By pumping nonresonantly a MoS$_2$ monolayer at $13$ K under a circularly polarized cw laser, we observe exciton energy redshifts that break the degeneracy between B excitons with opposite spin. The energy splitting increases monotonically with the laser power reaching as much as $18$ meV, while it diminishes with the temperature. The phenomenon can be explained theoretically by considering simultaneously the bandgap renormalization which gives rise to the redshift and exciton-exciton Coulomb exchange interaction which is responsible for the spin-dependent splitting. Our results offer a simple scheme to control the valley degree of freedom in MoS$_2$ monolayer and provide an accessible method in investigating many-body exciton exciton interaction in such materials.
The temperature-dependent optical response of excitons in semiconductors is controlled by the exciton-phonon interaction. When the exciton-lattice coupling is weak, the excitonic line has a Lorentzian profile resulting from motional narrowing, with a width increasing linearly with the lattice temperature $T$. In contrast, when the exciton-lattice coupling is strong, the lineshape is Gaussian with a width increasing sublinearly with the lattice temperature, proportional to $sqrt{T}$. While the former case is commonly reported in the literature, here the latter is reported for the first time, for hexagonal boron nitride. Thus the theoretical predictions of Toyozawa [Progr. Theor. Phys. 20, 53 (1958)] are supported by demonstrating that the exciton-phonon interaction is in the strong coupling regime in this Van der Waals crystal.
Exciton condensation in an electron-hole bilayer system of monolayer transition metal dichalcogenides is analyzed at three different levels of theory to account for screening and quasiparticle renormalization. The large effective masses of the transition metal dichalcogenides place them in a strong coupling regime. In this regime, mean field (MF) theory with either an unscreened or screened interlayer interaction predicts a room temperature condensate. Interlayer and intralayer interactions renormalize the quasiparticle dispersion, and this effect is included in a GW approximation. The renormalization reverses the trends predicted from the unscreened or screened MF theories. In the strong coupling regime, intralayer interactions have a large impact on the magnitude of the order parameter and its functional dependencies on effective mass and carrier density.
We present a model for exciton-plasmon coupling based on an energy exchange mechanism between quantum emitters (QE) and localized surface plasmons in metal-dielectric structures. Plasmonic correlations between QEs give rise to a collective state exchanging its energy cooperatively with a resonant plasmon mode. By defining carefully the plasmon mode volume for a QE ensemble, we obtain a relation between QE-plasmon coupling and a cooperative energy transfer rate that is expressed in terms of local fields. For a single QE near a sharp metal tip, we find analytically the enhancement factor for QE-plasmon coupling relative to QE coupling to a cavity mode. For QEs distributed in an extended region enclosing a plasmonic structure, we find that the ensemble QE-plasmon coupling saturates to a universal value independent of system size and shape, consistent with the experiment.
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