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Highly nonlinear trion-polaritons in a monolayer semiconductor

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 Added by Oleksandr Kyriienko
 Publication date 2019
  fields Physics
and research's language is English




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Highly nonlinear optical materials with strong effective photon-photon interactions (Kerr-like nonlinearity) are required in the development of novel quantum sources of light as well as for ultrafast and quantum optical signal processing circuitry. Here we report very large Kerr-like nonlinearities by employing strong optical transitions of charged excitons (trions) observed in semiconducting transition metal dichalcogenides (TMDCs). By hybridising trions in monolayer MoSe$_2$ at low electron densities with a microcavity mode, we realise trion-polaritons exhibiting significant energy shifts at very small photon fluxes due to phase space filling. Most notably, the strong trion-polariton nonlinearity is found to be 10 to 1000 larger than in other polariton systems, including neutral exciton-polaritons in TMDCs. Furthermore it exceeds by factors of $sim 10^3-10^5$ the magnitude of Kerr nonlinearity in bare TMDCs, graphene and other widely used optical materials (e.g. Si, AlGaAs etc) in weak light-matter coupling regimes. The results are in good agreement with a theory which accounts for the composite nature of excitons and trions and deviation of their statistics from that of ideal bosons and fermions. This work opens a new highly nonlinear system for quantum optics applications enabling in principle scalability and control through nano-engineering of van der Waals heterostructures.



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Two-dimensional transition metal dichalcogenide (TMD) semiconductors provide a unique possibility to access the electronic valley degree of freedom using polarized light, opening the way to valley information transfer between distant systems. Excitons with a well-defined valley index (or valley pseudospin) as well as superpositions of the exciton valley states can be created with light having circular and linear polarization, respectively. However, the generated excitons have short lifetimes (ps) and are also subject to the electron-hole exchange interaction leading to fast relaxation of the valley pseudospin and coherence. Here we show that control of these processes can be gained by embedding a monolayer of WSe$_2$ in an optical microcavity, where part-light-part-matter exciton-polaritons are formed in the strong light-matter coupling regime. We demonstrate the optical initialization of the valley coherent polariton populations, exhibiting luminescence with a linear polarization degree up to 3 times higher than that of the excitons. We further control the evolution of the polariton valley coherence using a Faraday magnetic field to rotate the valley pseudospin by an angle defined by the exciton-cavity-mode detuning, which exceeds the rotation angle in the bare exciton. This work provides unique insight into the decoherence mechanisms in TMDs and demonstrates the potential for engineering the valley pseudospin dynamics in monolayer semiconductors embedded in photonic structures.
Optical bound states in the continuum (BICs) provide a way to engineer very narrow resonances in photonic crystals. The extended interaction time in such systems is particularly promising for enhancement of nonlinear optical processes and development of the next generation of active optical devices. However, the achievable interaction strength is limited by the purely photonic character of optical BICs. Here, we mix optical BIC in a photonic crystal slab with excitons in atomically thin semiconductor MoSe$_2$ to form nonlinear exciton-polaritons with a Rabi splitting of 27~meV, exhibiting large interaction-induced spectral blueshifts. The asymptotic BIC-like suppression of polariton radiation into far-field towards the BIC wavevector, in combination with effective reduction of excitonic disorder through motional narrowing, results in small polariton linewidths below 3~meV. Together with strongly wavevector-dependent Q-factor, this provides for enhancement and control of polariton--polariton interactions and resulting nonlinear optical effects, paving the way towards tunable BIC-based polaritonic devices for sensing, lasing, and nonlinear optics.
The newly discovered valley degree of freedom (DOF) in atomically thin two-dimensional (2D) transition metal dichalcogenides (TMDs) offers a promising platform to explore rich nonlinear physics, such as spinor Bose-Einstein condensate (BEC) and novel valleytronics applications. However, the critical nonlinear effect, such as valley polariton bosonic stimulation (BS), has long remained an unresolved challenge due to the generation of limited polariton ground state densities necessary to induce the stimulated scattering of polaritons in specific valleys. Here, we report, for the first time, the valley bosonic stimulation of exciton-polaritons via spin-valley locking in a WS2 monolayer microcavity. This is achieved by the resonant injection of valley polaritons at specific energy and wavevector, which allows spin-polarized polaritons to efficiently populate their ground state and induce a valley-dependent bosonic stimulation. As a result, we observe the nonlinear self-amplification of polariton emission from the valley-dependent ground state. Our finding paves the way for both fundamental study of valley polariton BEC physics and non-linear optoelectronic devices such as spin-dependent parametric oscillators and spin-lasers.
274 - N. Lundt , P. Nagler , A. Nalitov 2017
Transition metal dichalcogenides represent an ideal testbed to study excitonic effects, spin-related phenomena and fundamental light-matter coupling in nanoscopic condensed matter systems. In particular, the valley degree of freedom, which is unique to such direct band gap monolayers with broken inversion symmetry, adds fundamental interest in these materials. Here, we implement a Tamm-plasmon structure with an embedded MoSe2 monolayer and study the formation of polaritonic quasi-particles. Strong coupling conditions between the Tamm-mode and the trion resonance of MoSe2 are established, yielding bright luminescence from the polaritonic ground state under non-resonant optical excitation. We demonstrate, that tailoring the electrodynamic environment of the monolayer results in a significantly increased valley polarization. This enhancement can be related to change in recombination dynamics shown in time-resolved photoluminescence measurements. We furthermore observe strong upconversion luminescence from resonantly excited polariton states in the lower polariton branch. This upconverted polariton luminescence is shown to preserve the valley polarization of the trion-polariton, which paves the way towards combining spin-valley physics and exciton scattering experiments.
Observations of polariton condensation in semiconductor microcavities suggest that polaritons can be exploited as a novel type of laser with low input-power requirements. The low-excitation regime is approximately equivalent to thermal equilibrium, and a higher excitation results in more dominant nonequilibrium features. Although standard photon lasing has been experimentally observed in the high excitation regime, e-h pair binding can still remain even in the high-excitation regime theoretically. Therefore, the photoluminescence with a different photon lasing mechanism is predicted to be different from that with a standard photon lasing. In this paper, we report the temperature dependence of the change in photoluminescence with the excitation density. The second threshold behavior transited to the standard photon lasing is not measured at a low-temperature, high-excitation power regime. Our results suggest that there may still be an electron--hole pair at this regime to give a different photon lasing mechanism.
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