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The sequential resonant excitation of a 2-level quantum system results in the emission of a state of light showing time-entanglement encoded in the photon-number-basis - notions that can be extended to 3-level quantum systems as discussed in a recent proposal. Here, we report the experimental implementation of a sequential two-photon resonant excitation process of a solid-state 3-level system, constituted by the biexciton-, exciton-, and ground-state of a semiconductor quantum dot. The resulting light state exhibits entanglement in time and energy, encoded in the photon-number basis, which could be used in quantum information applications, e.g., dense information encoding or quantum communication protocols. Performing energy- and time-resolved correlation experiments in combination with extensive theoretical modelling, we are able to partially retrieve the entanglement structure of the generated state., Comment: 14 pages (including 5 figures, 56 citations)

Bosonic condensation and lasing of exciton-polaritons in microcavities is a fascinating solid-state phenomenon. It provides a versatile platform to study out-of-equilibrium many-body physics and has recently appeared at the forefront of quantum technologies. Here, we study the photon statistics via the second-order temporal correlation function of polariton lasing emerging from an optical microcavity integrated with an atomically thin MoSe2 crystal. Furthermore, we investigate the macroscopic polariton phase transition for varying excitation powers and temperatures. The lower-polariton exhibits photon bunching below the threshold, implying a dominant thermal distribution of the emission, while above the threshold, the second-order correlation transits towards unity, which evidences the formation of a coherent state. Our findings are in agreement with a microscopic numerical model, which explicitly includes scattering with phonons on the quantum level., Comment: This manuscript was published in Phys. Rev. Lett., see https://journals.aps.org/prl/abstract/10.1103/PhysRevLett.131.206901

In this review, we describe the current landscape of emergent quantum materials for quantum photonic applications. We focus on three specific solid-state platforms: single emitters in monolayers of transition metal dichalcogenides, defects in hexagonal boron nitride, and colloidal quantum dots in perovskites. These platforms share a unique technological accessibility, enabling the rapid implementation of testbed quantum applications, all while being on the verge of becoming technologically mature enough for a first generation of real-world quantum applications. The review begins with a comprehensive overview of the current state-of-the-art for relevant single-photon sources in the solid-state, introducing the most important performance criteria and experimental characterization techniques along the way. We then benchmark progress for each of the three novel materials against more established (yet complex) platforms, highlighting performance, material-specific advantages, and giving an outlook on quantum applications. This review will thus provide the reader with a snapshot on latest developments in the fast-paced field of emergent single-photon sources in the solid-state, including all the required concepts and experiments relevant to this technology., Comment: 35 pages, 8 figures, review paper

In recent years, much research has been undertaken to investigate the suitability of two-dimensional materials to act as single-photon sources with high optical and quantum optical quality. Amongst them, transition-metal dichalcogenides, especially WSe$_{2}$, have been one of the subjects of intensive studies. Yet, their single-photon purity and photon indistinguishability, remain the most significant challenges to compete with mature semiconducting systems such as self-assembled InGaAs quantum dots. In this work, we explore the emission properties of quantum emitters in a WSe$_{2}$ monolayer which are induced by metallic nanoparticles. Under quasi-resonant pulsed excitation, we verify clean single-photon emission with a $g^{(2)}(0) = 0.036\pm0.004$. Furthermore, we determine its temperature dependent coherence time via Michelson interferometry, where a value of (13.5$\pm$1.0) ps is extracted for the zero-phonon line (ZPL) at 4 K, which reduces to (9$\pm$2) ps at 8 K. Associated time-resolved photoluminescence experiments reveal a decrease of the decay time from (2.4$\pm$0.1) ns to (0.42$\pm$0.05) ns. This change in decay time is explained by a model which considers a F\"orster-type resonant energy transfer process, which yields a strong temperature induced energy loss from the SPE to the nearby Ag nanoparticle.

Emitter dephasing is one of the key issues in the performance of solid-state single photon sources. Among the various sources of dephasing, acoustic phonons play a central role in adding decoherence to the single photon emission. Here, we demonstrate, that it is possible to tune and engineer the coherence of photons emitted from a single WSe$_2$ monolayer quantum dot via selectively coupling it to a spectral cavity resonance. We utilize an open cavity to demonstrate spectral enhancement, leveling, and suppression of the highly asymmetric phonon sideband, finding excellent agreement with a microscopic description of the exciton-phonon dephasing in a truly two-dimensional system. Moreover, the impact of cavity tuning on the dephasing is directly assessed via optical interferometry, which points out the capability to utilize light-matter coupling to steer and design dephasing and coherence of quantum emitters in atomically thin crystals.

We propose a general scheme to generate entanglement encoded in the photon-number basis, via a sequential resonant two-photon excitation of a three-level system. We apply it to the specific case of a quantum dot three-level system, which can emit a photon pair through a biexciton-exciton cascade. The state generated in our scheme constitutes a tool for secure communication, as the multipartite correlations present in the produced state may provide an enhanced rate of secret communication with respect to a perfect GHZ state., Comment: 05 pages and 04 figures

We revisit and extend the standard bosonic interpretation of interlayer excitons in the moir\'e potential of twisted heterostructures of transition-metal dichalcogenides. In our experiments, we probe a high quality MoSe$_2$/WSe$_2$ van der Waals bilayer heterostructure via density-dependent photoluminescence spectroscopy and reveal strongly developed, unconventional spectral shifts of the emergent moir\'e exciton resonances. The observation of saturating blueshifts of successive exciton resonances allow us to explain their physics in terms of a model utilizing fermionic saturable absorbers. This approach is strongly inspired by established quantum-dot models, which underlines the close analogy of interlayer excitons trapped in pockets of the moir\'e potential, and quantum emitters with discrete eigenstates.

Solid-state single photon sources are central building blocks in quantum communication networks and on-chip quantum information processing. Atomically thin crystals were established as possible candidates to emit non-classical states of light, however, the performance of monolayer-based single photon sources has so far been lacking behind state-of-the-art devices based on volume crystals. Here, we implement a single photon source based on an atomically thin sheet of WSe2 coupled to a spectrally tunable optical cavity. It is characterized by a high single photon purity with a $g^{(2)}(0)$ value as low as $4.7 \pm 0.7 \%$ and a record-high first lens brightness of linearly polarized photons as large as $65 \pm 4 \%$. Interestingly, the high performance of our devices allows us to observe genuine quantum interference phenomena in a Hong-Ou-Mandel experiment. Our results demonstrate that open cavities and two-dimensional materials constitute an excellent platform for ultra-bright quantum light sources: the unique properties of such two-dimensional materials and the versatility of open cavities open an inspiring avenue for novel quantum optoelectronic devices., Comment: 12 pages, 7 figures

Engineering the properties of quantum materials via strong light-matter coupling is a compelling research direction with a multiplicity of modern applications. Those range from modifying charge transport in organic molecules, steering particle correlation and interactions, and even controlling chemical reactions. Here, we study the modification of the material properties via strong coupling and demonstrate an effective inversion of the excitonic band-ordering in a monolayer of WSe2 with spin-forbidden, optically dark ground state. In our experiments, we harness the strong light-matter coupling between cavity photon and the high energy, spin-allowed bright exciton, and thus creating two bright polaritonic modes in the optical bandgap with the lower polariton mode pushed below the WSe2 dark state. We demonstrate that in this regime the commonly observed luminescence quenching stemming from the fast relaxation to the dark ground state is prevented, which results in the brightening of this intrinsically dark material. We probe this effective brightening by temperature-dependent photoluminescence, and we find an excellent agreement with a theoretical model accounting for the inversion of the band ordering and phonon-assisted polariton relaxation.

To date, quantum communication widely relies on attenuated lasers for secret key generation. In future quantum networks fundamental limitations resulting from their probabilistic photon distribution must be overcome by using deterministic quantum light sources. Confined excitons in monolayers of transition metal dichalcogenides (TMDCs) constitute an emerging type of emitter for quantum light generation. These atomically-thin solid-state sources show appealing prospects for large-scale and low-cost device integration, meeting the demands of quantum information technologies. Here, we pioneer the practical suitability of TMDC devices in quantum communication. We employ a $\mathrm{WSe}_2$ monolayer single-photon source to emulate the BB84 protocol in a quantum key distribution (QKD) setup and achieve click rates of up to 66.95 kHz and antibunching values down to 0.034 - a performance competitive with QKD experiments using semiconductor quantum dots or color centers in diamond. Our work opens the route towards wider applications of quantum information technologies using TMDC single-photon sources., Comment: Main text: 11 pages (including 4 figures, 1 table, and 58 citations); Supplementary: 5 pages (including 6 figures) Revised version with extended discussions of the results in the main text and extended information in the supplementary

The optical properties of monolayer transition metal dichalcogenides are dominated by tightly-bound excitons. They form at distinct valleys in reciprocal space, and can interact via the valley-exchange coupling, modifying their dispersion considerably. Here, we predict that angle-resolved photoluminescence can be used to probe the changes of the excitonic dispersion. The exchange-coupling leads to a unique angle dependence of the emission intensity for both circularly and linearly-polarised light. We show that these emission characteristics can be strongly tuned by an external magnetic field due to the valley-specific Zeeman-shift. We propose that angle-dependent photoluminescence measurements involving both circular and linear optical polarisation as well as magnetic fields should act as strong verification of the role of valley-exchange coupling on excitonic dispersionand its signatures in optical spectra

The emergence of spatial and temporal coherence of light emitted from solid-state systems is a fundamental phenomenon, rooting in a plethora of microscopic processes. It is intrinsically aligned with the control of light-matter coupling, and canonical for laser oscillation. However, it also emerges in the superradiance of multiple, phase-locked emitters, and more recently, coherence and long-range order have been investigated in bosonic condensates of thermalized light, as well as in exciton-polaritons driven to a ground state via stimulated scattering. Here, we experimentally show that the interaction between photons in a Fabry-Perot microcavity and excitons in an atomically thin WSe$_2$ layer is sufficient such that the system enters the hybridized regime of strong light-matter coupling at ambient conditions. Via Michelson interferometry, we capture clear evidence of increased spatial and temporal coherence of the emitted light from the spatially confined system ground-state. The coherence build-up is accompanied by a threshold-like behaviour of the emitted light intensity, which is a fingerprint of a polariton laser effect. Valley-physics is manifested in the presence of an external magnetic field, which allows us to manipulate K and K' polaritons via the Valley-Zeeman-effect. Our findings are of high application relevance, as they confirm the possibility to use atomically thin crystals as simple and versatile components of coherent light-sources, and in valleytronic applications at room temperature., Comment: 13 pages, 4 figures

Engineering non-linear hybrid light-matter states in tailored optical lattices is a central research strategy for the simulation of complex Hamiltonians. Excitons in atomically thin crystals are an ideal active medium for such purposes, since they couple strongly with light and bear the potential to harness giant non-linearities and interactions while presenting a simple sample-processing and room temperature operability. We demonstrate lattice polaritons, based on an open, high-quality optical cavity, with an imprinted photonic lattice strongly coupled to excitons in a WS$_{2}$ monolayer. We experimentally observe the emergence of the canonical band-structure of particles in a one-dimensional lattice at room temperature, and demonstrate frequency reconfigurability over a spectral window exceeding 12 meV, as well as the systematic variation of the nearest neighbour coupling, reflected by a tuneability in the bandwidth of the p-band polaritons by 7 meV. The technology presented in this work is a critical demonstration towards reconfigurable photonic emulators operated with non-linear photonic fluids, offering a simple experimental implementation and working at ambient conditions.

The emergence of two-dimensional crystals has revolutionized modern solid-state physics. From a fundamental point of view, the enhancement of charge carrier correlations has sparked enormous research activities in the transport- and quantum optics communities. One of the most intriguing effects, in this regard, is the bosonic condensation and spontaneous coherence of many-particle complexes. Here, we find compelling evidence of bosonic condensation of exciton-polaritons emerging from an atomically thin crystal of MoSe2 embedded in a dielectric microcavity under optical pumping. The formation of the condensate manifests itself in a sudden increase of luminescence intensity in a threshold-like manner, and a significant spin-polarizability in an externally applied magnetic field. Spatial coherence is mapped out via highly resolved real-space interferometry, revealing a spatially extended condensate. Our device represents a decisive step towards the implementation of coherent light-sources based on atomically thin crystals, as well as non-linear, valleytronic coherent devices., Comment: Main text: 11 pages, 5 figures, Supplementary Materials: 4 pages, 5 figures