Highly nonlinear trion-polaritons in a monolayer semiconductor

Abstract

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.

7 pages of the main text, and 26 pages of supplemental materials (details of the experiment and full theory description). Please also see the quantum theory in arXiv:1910.11294

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• Twist Angle Tuning of Moiré Exciton Polaritons in van der Waals Heterostructures
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• Exciton-Trion-Polaritons in Two-Dimensional Materials
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• Strong photon interactions from weakly interacting particles
• Electrostatic control of nonlinear photonic-crystal polaritons in a monolayer semiconductor
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• Microscopic theory of nonlinear phase space filling in polaritonic lattices
• Two-dimensional exciton-polariton interactions beyond the Born approximation
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• Efficient calculation of trion energies in monolayer transition metal dichalcogenides
• Theory of nonlinear excitonic response of hybrid organic perovskites in the regime of strong light-matter coupling
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• Polaritonic Machine Learning for Graph-based Data Analysis
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• Quantization of Polaritons Confined in Dielectric Structures