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Unique Light-Matter Interactions with Two-Dimensional Materials

Periodic Reporting for period 5 - unLiMIt-2D (Unique Light-Matter Interactions with Two-Dimensional Materials)

Période du rapport: 2022-11-01 au 2023-10-31

Controlling light- and matter excitations down to the microscopic scale is one major challenge in modern optics. Applications arising from this field, such as novel coherent- and quantum light sources have the potential to affect our daily life. One particularly appealing material platform in quantum physics consists of monolayer crystals. The most prominent species, graphene, however remains rather unappealing for photonic applications due to the lack of an electronic bandgap in its pristine form. Monolayers of transition metal dichalcogenides and group III-VI compounds comprise such a direct bandgap, and additionally feature intriguing spinor properties, making them almost ideal candidates to study optics and excitonic effects in two-dimensional systems.
unLiMIt-2D aims to establish these materials as a new platform in solid-state cavity quantum electrodynamics. The targeted experiments will be based on thin layers embedded in high quality photonic heterostructures providing optical confinement.
unLiMIt-2D will exploit the combination of ultra-large exciton binding energies, giant absorption and unique spin properties of such materials to form microcavity exciton polaritons. These composite bosons provide the unique possibility to study coherent quantum fluids up to room temperature. Due to the possibility of fabricating such structures by relatively simple means, establishing bosonic condensation effects in atomic monolayers can lead to a paradigm shift in polaritonics.
Secondly, the project will focus on exciton localization in layered materials, with the perspective to establish a new generation of microcavity-based quantum light sources. Light-matter coupling effects will greatly improve the performance of such sources.

Within the ERC action, the potential of TMD monlayers in polaritonics was established, verified by the successful demonstrations of room-temperature strong coupling, as well as the condensation of polaritons from 3K to 300K. Furthermore, the action has established WSe2 monolayers as a promising candidate for high-performance, scalable single photon sources.
Within the first twp reporting periods, the PI and his Team have concluded a variety of breakthrough results in the field light-matter coupling with atomically thin materials. The Team could show, that it is possible to reach the strong coupling Regime of exciton and Photons in a microcavity with a single embedded monolayer (N. Lundt et al. 10.1038/ncomms13328) and they demonstrated the valley selective strong coupling at cryogenic, (N. Lundt et al. 2D Materials 10.1088/2053-1583/aa6ef2) as well as at room temperature (N. Lundt et al. Physical Review B 10.1103/physrevb.96.241403). The Team furthermore demonstrated the formation of so-called hybrid polaritons composed of III-V and TMDC excitons (M. Wurdack et al. Nature Communications 10.1038/s41467-017-00155-w) and subsequently the bosonic condensation of exciton-polaritons in a hybrid cavity at cryogenic temperature (M. Waldherr et al. Nature Communications 10.1038/s41467-018-05532-7).

The ERC Team identified techniques to Isolate single excitons in WSe2 monolayers via strain engineering (O. Iff et al. Optics Express 10.1364/oe.26.025944) and subsequently, the coupling of a strain-localized single exciton (single photon sources) to a plasmonic resonance (L. Tripathi et al. ACS Photonics 10.1021/acsphotonics.7b01053). Further, the team demonstrated the formation of biexciton states via quantum corelations (He et al. Nature Communications 10.1038/ncomms13409 28).
Among the major achievements in the third reporting period, the novel Valley Hall Effect of Exciton Polaritons (Lundt et al. Nature Nanotechnology 14 770 (2019)) , the initial demonstration of Valley Zeeman Splitting of TMD polaritons (Klaas et al. PRB 100 121303 (2019)) and full control over the effect of valley coherence in real- and artificial magnetic fields (Rupprecht et al. 2D Materials 7 035025 (2020)) were reported. We have furthermore reported giant strain-tuneability of TMD-based single photon sources (Iff et al. Nanoletters 19 6931 (2019)).

During the fourth reporting period we have demonstrated the first condensation of exciton-polaritons using TMDC monolayer in Nature Materials at cryogenic temperatures (Anton-Solanas et al. Nature Materials 20 1233 (2021)) as well as the coherence of exciton-polaritons at room temperature (M2.3) (Shan et al. Nature Communications 12, 6406 (2021)) . We furthermore observed the the surprising phenomena of polariton induced triplet quenching (or exciton brightening), (Shan et al. Nature Communications 13 3001 (2022)) . Finally, our technological developments of tunable open cavities have allowed us to demonstrate fully tunable polaritons in photonic lattices at room temperature (Lackner et al. Nature Communications 12, 4933 (2021)). We have furthermore reported the successful realization of TMDC-based single photon sources using the strain-positioning technique in combination with lateral Bragg-grating cavities (Iff et al. Nanoletters 21 4715 (2021)) (corresponding Milestones M3.2.2 and M3.3).

The following major scientific achievements were accomplished in the final reporting period (PR5), and successfully published and disseminated in peer review articles:

Following our demonstration of spatial coherence of exciton-polaritons, both at cryogenic conditions as well as at room temperature in the fourth reporting period , we were able to proof quantum coherence in a polariton system in the fifth period. The effect was demonstrated via the Hanbury-Brown and Twiss experiment, which allowed us to reconstruct the second order correlation function of the emitted light from our polariton fluid. The paper was published in Physical Review Letters in 2023. (Shan et al. Physical review Letters 131, 206901 (2023))

We have furthermore reported the successful realization of TMDC-based single photon sources in our open, tunable microcavity. The paper marks the state-of-the-art in the field, demonstrating high brightness, high purity quantum emission, and finally quantum coherence of single photons emitted by WSe2 quantum dot. T (Drawer, Mitryakhin, Shan et al. Nanoletters 23, 8683 (2023)). The soruce performance was directly exploited in the first quantum communication demonstration utilizing transition metal dichalcogenides, in collaboration with the group of T. Heindel at TU Berlin (Gao et al. NJP 2D Materials and their applications (2023))
The results indicated in the section above indeed all go well beyond the state of the art, yielding original journal publications. Altogether, within the project, more than 30 peer reviewed papers were published by the team.
The demonstrations of hybrid bosonic condensation in a microcavity with a monolayer crystal (M. Waldherr et al. Nature Communications 10.1038/s41467-018-05532-7) as well as the condensation of TMD polaritons at cryogenic and finally at room temperature are considered as a landmark experiment for the field. They stringently established TMD materials as one of the main platforms of cavity quantum electrodynamics and polaritonics.

On the other hand, while the ERC team has progressively pushed the field of single photon sources based on WSe2 monolayers. After the initial demonstrations of light-matter coupling of WSe2 quantum dots using metallic surfaces, the strain tunability, as well as the emission of single photons in the regime of high Purcell enhancement were all published by the ERC team. With the conclusion of the ERC activity, WSe2 monolayer quantum dots are nowadays used in applied quantum technological applications, such as quantum secured communications.
Schematic drawing and photograph of an optical microcavity wtih embedded TMD crystal.