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      Revealing Strong Plasmon-Exciton Coupling Between Nano-gap Resonators and Two-Dimensional Semiconductors at Ambient Conditions

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          Abstract

          Strong coupling of two-dimensional semiconductor excitons with plasmonic resonators enables control of light-matter interaction at the subwavelength scale. Here we develop strong coupling in plasmonic nano-gap resonators that allow modification of exciton number contributing to the coupling. Using this system, we not only demonstrate a large vacuum Rabi splitting up to 163 meV and splitting features in photoluminescence spectra, but also reveal that the exciton number can be reduced down to single-digit level (N<10), which is an order lower than that of traditional systems, close to single-exciton based strong coupling. In addition, we prove that the strong coupling process is not affected by the large exciton coherence size that was previously believed to be detrimental to the formation of plasmon-exciton interaction. Our work provides a deeper understanding of storng coupling in two-dimensional semiconductors, paving the way for room temperature quantum optics applications.

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          Quantum nature of a strongly-coupled single quantum dot-cavity system

           ,  ,   (2006)
          Cavity quantum electrodynamics (QED) studies the interaction between a quantum emitter and a single radiation-field mode. When an atom is in strong coupling with a cavity mode1,2, it is possible to realize key quantum information processing (QIP) tasks, such as controlled coherent coupling and entanglement of distinguishable quantum systems. Realizing these tasks in the solid state is clearly desirable, and coupling semiconductor self-assembled quantum dots (QDs) to monolithic optical cavities is a promising route to this end. However, validating the efficacy of QDs in QIP applications requires confirmation of the quantum nature of the QD-cavity system in the strong coupling regime. Here we find a confirmation by observing quantum correlations in photoluminescence (PL) from a photonic crystal (PC) nanocavity3-5 interacting with one, and only one, QD located precisely at the cavity electric field maximum. When off-resonance, photon emission from the cavity mode and QD excitons is anti-correlated at the level of single quanta, proving that the mode is driven solely by the QD despite an energy mis-match between cavity and excitons. When tuned into resonance, the exciton and photon enter the strong-coupling regime of cavity-QED and the QD lifetime reduces by a factor of 120. The photon stream from the cavity becomes anti-bunched, proving that the coupled exciton/photon system is in the quantum anharmonic regime. Our observations unequivocally show that QIP tasks requiring the quantum nonlinear regime are achievable in the solid state.
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            Probing Excitonic Dark States in Single-layer Tungsten Disulfide

            Transition metal dichalcogenide (TMDC) monolayer has recently emerged as an important two-dimensional semiconductor with promising potentials for electronic and optoelectronic devices. Unlike semi-metallic graphene, layered TMDC has a sizable band gap. More interestingly, when thinned down to a monolayer, TMDC transforms from an indirect bandgap to a direct bandgap semiconductor, exhibiting a number of intriguing optical phenomena such as valley selective circular dichroism, doping dependent charged excitons, and strong photocurrent responses. However, the fundamental mechanism underlying such a strong light-matter interaction is still under intensive investigation. The observed optical resonance was initially considered to be band-to-band transitions. In contrast, first-principle calculations predicted a much larger quasiparticle band gap size and an optical response that is dominated by excitonic effects. Here, we report experimental evidence of the exciton dominance mechanism by discovering a series of excitonic dark states in single-layer WS2 using two-photon excitation spectroscopy. In combination with GW-BSE theory, we find the excitons are Wannier excitons in nature but possess extraordinarily large binding energy (~0.7 eV), leading to a quasiparticle band gap of 2.7 eV. These strongly bound exciton states are observed stable even at room temperature. We reveal an exciton series in significant deviation from hydrogen models, with a novel inverse energy dependence on the orbital angular momentum. These excitonic energy levels are experimentally found robust against environmental perturbations. The discovery of excitonic dark states and exceptionally large binding energy not only sheds light on the importance of many-electron effects in this two-dimensional gapped system, but also holds exciting potentials for the device application of TMDC monolayers and their heterostructures.
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              Observation of Mode Splitting in Photoluminescence of Individual Plasmonic Nanoparticles Strongly Coupled to Molecular Excitons

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                Author and article information

                Journal
                05 November 2018
                Article
                1811.01598

                http://arxiv.org/licenses/nonexclusive-distrib/1.0/

                Custom metadata
                physics.optics cond-mat.mes-hall

                Nanophysics, Optical materials & Optics

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