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Two-dimensional semiconductors in the regime of strong light-matter coupling

Published 18 Apr 2018 in cond-mat.mes-hall and cond-mat.mtrl-sci | (1804.06771v1)

Abstract: The optical properties of transition metal dichalcogenide monolayers are widely dominated by excitons, Coulomb-bound electron-hole pairs. These quasi-particles exhibit giant oscillator strength and give rise to narrow-band, well-pronounced optical transitions, which can be brought into resonance with electromagnetic fields in microcavities and plasmonic nanostructures. Due to the atomic thinness and robustness of the monolayers, their integration in van der Waals heterostructures provides unique opportunities for engineering strong light-matter coupling. We review first results in this emerging field and outline future opportunities and challenges.

Citations (307)

Summary

  • The paper demonstrates that strong exciton-light coupling in TMDC monolayers leads to the formation of exciton-polaritons and observable Rabi splitting.
  • It employs experimental setups with dielectric and metallic cavities alongside a coupled oscillator model to characterize optical phenomena.
  • The findings pave the way for developing valleytronic devices and quantum photonic applications by leveraging the unique spin-valley dynamics of excitons.

Two-Dimensional Semiconductors in the Regime of Strong Light-Matter Coupling

The paper explores the intriguing domain of two-dimensional transition metal dichalcogenides (TMDCs) and their substantial interactions with light within the strong-coupling regime. These interactions primarily involve excitons, which are electron-hole pairs tightly bound by Coulomb forces. The authors provide a comprehensive review of the optical properties of TMDC monolayers and the emerging phenomenon of strong light-matter coupling, offering insights into both experimental implementations and theoretical frameworks.

Key Optical Properties

TMDC monolayers display pronounced exciton resonances, even at ambient temperature, largely attributed to high exciton binding energies in the range of several hundred meV. This results in significant optical characteristics, such as high exciton oscillator strength—capable of absorbing up to 20% of incident light per monolayer—and radiative lifetimes within the 100 fs to several ps range. The strong coupling between these excitons and light gives rise to exciton-polaritons, composite particles exhibiting characteristics of both matter and light. The valley-selective dipole selection rules in TMDCs, combined with substantial spin-orbit coupling, facilitate explorations into spin-valley dynamics of excitons.

Strong Light-Matter Coupling Phenomenon

Strong light-matter coupling is investigated through the integration of excitons with photon modes within microcavities and plasmonic structures. This coupling produces exciton-polaritons, altering emission characteristics and resulting in phenomena such as Rabi splitting in the spectral domain. The strong coupling regime is defined by scenarios where coherent energy exchange between excitons and optical modes prevails over their respective decay processes. Theoretical descriptions are often based on coupled oscillators models, and experimental observations typically involve identifying an anti-crossing in energy spectra as a function of cavity-exciton detuning.

Experimental Implementations

Various designs have been employed to achieve strong coupling conditions at both cryogenic and room temperatures. Initial experiments using dielectric distributed Bragg reflectors (DBRs) with TMDC monolayers embedded within yielded proof-of-concept results. Metallic cavities and plasmonic structures offer alternative configurations with reduced mode volumes, aiming to enhance the coupling strength. Despite challenges such as inhomogeneous broadening and fabrication complexities, devices exhibiting clear exciton-polariton characteristics have been developed. A noteworthy approach involves hybrid polariton systems combining inorganic and organic excitons, potentially enhancing interaction dynamics and enabling advanced photonic applications.

Implications and Future Directions

The theoretical insights and experimental validations within the paper highlight potential trajectories for further research. Strong light-matter coupling in 2D TMDCs paves the way for future investigations into polaritonic Bose-Einstein condensates and superfluidity. The valley-selective exciton dynamics offer prospects for valleytronic devices, where valley polarization can be harnessed for information processing. Additionally, integrating TMDCs with chiral cavities could facilitate novel phenomena such as chiral lasing.

The exploration of TMDCs in the strong-coupling regime reveals not only fundamental photophysical processes but also promises a broad spectrum of technological advancements in the fields of high-speed optical communication, low-power switching, and quantum computing. The synergy between material science and quantum optics continues to uncover unprecedented pathways, laying the groundwork for innovative device architectures and multifunctional photonic platforms.

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