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Register a new userNonclassical Light from Exciton Interactions in a Two-Dimensional Quantum Mirror
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Excitons in a semiconductor monolayer form a collective resonance that can reflect resonant light with extraordinarily high efficiency. Here, we investigate the nonlinear optical properties of such atomistically thin mirrors and show that finite-range interactions between excitons can lead to the generation of highly non-classical light. We describe two scenarios, in which optical nonlinearities arise either from direct photon coupling to excitons in excited Rydberg states or from resonant two-photon excitation of Rydberg excitons with finite-range interactions. The latter case yields conditions of electromagnetically induced transparency and thereby provides an efficient mechanism for single-photon switching between high transmission and reflectance of the monolayer, with a tunable dynamical timescale of the emerging photon-photon interactions. Remarkably, it turns out that the resulting high degree of photon correlations remains virtually unaffected by Rydberg-state decoherence, in excess of non-radiative decoherence observed for ground-state excitons in two-dimensional semiconductors. This robustness to imperfections suggests a promising new approach to quantum photonics at the level of individual photons.
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The on-chip generation of non-classical states of light is a key-requirement for future optical quantum hardware. In solid-state cavity quantum electrodynamics, such non-classical light can be generated from self-assembled quantum dots strongly coupled to photonic crystal cavities. Their anharmonic strong light-matter interaction results in large optical nonlinearities at the single photon level, where the admission of a single photon into the cavity may enhance (photon-tunnelling) or diminish (photon-blockade) the probability for a second photon to enter the cavity. Here, we demonstrate that detuning the cavity and QD resonances enables the generation of high-purity non-classical light from strongly coupled systems. For specific detunings we show that not only the purity but also the efficiency of single-photon generation increases significantly, making high-quality single-photon generation by photon-blockade possible with current state-of-the-art samples.
Coherent coupling between excitons is at the heart of many-body interactions with transition metal dichalcogenide (TMD) heterostructures as an emergent platform for the investigation of these interactions. We employ multi-dimensional coherent spectroscopy on monolayer MoSetextsubscript{2}/WSetextsubscript{2} heterostructures and observe coherent coupling between excitons spatially localized in monolayer MoSe$_2$ and WSe$_2$. Through many-body spectroscopy, we further observe the absorption state arising from free interlayer electron-hole pairs. This observation yields a spectroscopic measurement of the interlayer exciton binding energy of about 250 meV.
We experimentally demonstrate time-resolved exciton propagation in a monolayer semiconductor at cryogenic temperatures. Monitoring phonon-assisted recombination of dark states, we find a highly unusual case of exciton diffusion. While at 5 K the diffusivity is intrinsically limited by acoustic phonon scattering, we observe a pronounced decrease of the diffusion coefficient with increasing temperature, far below the activation threshold of higher-energy phonon modes. This behavior corresponds neither to well-known regimes of semiclassical free-particle transport nor to the thermally activated hopping in systems with strong localization. Its origin is discussed in the framework of both microscopic numerical and semi-phenomenological analytical models illustrating the observed characteristics of nonclassical propagation. Challenging the established description of mobile excitons in monolayer semiconductors, these results open up avenues to study quantum transport phenomena for excitonic quasiparticles in atomically-thin van der Waals materials and their heterostructures.
Despite tremendous advances in the fundamentals and applications of cavity quantum electrodynamics (CQED), investigations in this field have primarily been limited to optical cavities composed of purely dielectric materials. Here, we demonstrate a hybrid metal-dielectric nanocavity design and realize it in the InAs/GaAs quantum photonics platform utilizing angled rotational metal evaporation. Key features of our nanometallic light-matter interface include: (i) order of magnitude reduction in mode volume compared to that of leading photonic crystal CQED systems; (ii) surface-emitting nanoscale cylindrical geometry and therefore good collection efficiency; and finally (iii) strong and broadband spontaneous emission rate enhancement (Purcell factor ~ 8) of single photons. This light-matter interface may play an important role in quantum technologies.
Strong many-body interactions in two-dimensional (2D) semiconductors give rise to efficient exciton-exciton annihilation (EEA). This process is expected to result in the generation of unbound high energy carriers. Here, we report an unconventional photoresponse of van der Waals heterostructure devices resulting from efficient EEA. Our heterostructures, which consist of monolayer transition metal dichalcogenide (TMD), hexagonal boron nitride (hBN), and few-layer graphene, exhibit photocurrent when photoexcited carriers possess sufficient energy to overcome the high energy barrier of hBN. Interestingly, we find that the device exhibits moderate photocurrent quantum efficiency even when the semiconducting TMD layer is excited at its ground exciton resonance despite the high exciton binding energy and large transport barrier. Using ab initio calculations, we show that EEA yields highly energetic electrons and holes with unevenly distributed energies depending on the scattering condition. Our findings highlight the dominant role of EEA in determining the photoresponse of 2D semiconductor optoelectronic devices.
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