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Preprints
197. A. de la Torre, D. M. Kennes, E. Malic, S. Kar „Review: Spatial inhomogeneities, moiré potential and moiré excitons”, arXiv: 2402.19236
In this short review, we provide an overview of recent progress in deploying advanced characterization techniques to understand the effects of local inhomogeneities in moiré heterostructures over multiple length scales. Particular emphasis is placed on correlating the impact of twist angle misalignment, nano-scale disorder, and atomic relaxation on the moiré potential and its collective excitations, particularly moiré excitons. Finally, we discuss future technological applications leveraging based on moié excitons.
arXiv: 2402.19236196. B. Ferreira, H. Shan, R. Rosati, J. M. Fitzgerald, L. Lackner, B. Han, M. Esmann, P. Hays, G. Liebling, K. Watanabe, T. Taniguchi, F. Eilenberger, S. Tongay, C. Schneider, E. Malic, "Revealing dark exciton signatures in polariton spectra of 2D materials", arXiv: 2401.04588
Dark excitons in transition metal dichalcogenides (TMD) have been so far neglected in the context of polariton physics due to their lack of oscillator strength. However, in tungsten-based TMDs, dark excitons are known to be the energetically lowest states and could thus provide important scattering partners for polaritons. In this joint theory-experiment work, we investigate the impact of the full exciton energy landscape on polariton absorption and reflectance. By changing the cavity detuning, we vary the polariton energy relative to the unaffected dark excitons in such a way that we open or close specific phonon-driven scattering channels. We demonstrate both in theory and experiment that this controlled switching of scattering channels manifests in characteristic sharp changes in optical spectra of polaritons. These spectral features can be exploited to extract the position of dark excitons. Our work suggests new possibilities for exploiting polaritons for fingerprinting nanomaterials via their unique exciton landscape.
arXiv: 2401.04588195. J. M. Fitzgerald, R. Rosati, B. Ferreira, H. Shan, C. Schneider, E. Malic, "Circumventing the polariton bottleneck via dark excitons in 2D semiconductors", arXiv: 2401.03825v1
Efficient scattering into the exciton polariton ground state is a key prerequisite for generating Bose-Einstein condensates and low-threshold polariton lasing. However, this can be challenging to achieve at low densities due to the polariton bottleneck effect that impedes phonon-driven scattering into low-momentum polariton states. The rich exciton landscape of transition metal dichalcogenides (TMDs) provides potential intervalley scattering pathways via dark excitons to rapidly populate these polaritons. Here, we present a microscopic study exploring the time- and momentum-resolved relaxation of exciton polaritons supported by a \ce{MoSe2} monolayer integrated within a Fabry-Perot cavity. By exploiting phonon-assisted transitions between momentum-dark excitons and the lower polariton branch, we demonstrate that it is possible to circumvent the bottleneck region and efficiently populate the polariton ground state. Furthermore, this intervalley pathway is predicted to give rise to, yet unobserved, angle-resolved phonon sidebands in low-temperature photoluminescence spectra that are associated with momentum-dark excitons. This represents a distinctive experimental signature for efficient phonon-mediated polariton-dark-exciton interactions.
arXiv: 2401.03825v1194. A. Kumar, D. Yagodkin, R. Rosati, D. J Bock, C. Schattauer, S. Tobisch, J. Hagel, B. Höfer, J. N Kirchhof, P. Hernández López, K. Burfeindt, S. Heeg, C. Gahl, F. Libisch, E. Malic, K. I Bolotin “Strain fingerprinting of exciton valley character”, arXiv: 2312.07332
Momentum-indirect excitons composed of electrons and holes in different valleys define optoelectronic properties of many semiconductors, but are challenging to detect due to their weak coupling to light. The identification of an excitons' valley character is further limited by complexities associated with momentum-selective probes. Here, we study the photoluminescence of indirect excitons in controllably strained prototypical 2D semiconductors (WSe2, WS2) at cryogenic temperatures. We find that these excitons i) exhibit valley-specific energy shifts, enabling their valley fingerprinting, and ii) hybridize with bright excitons, becoming directly accessible to optical spectroscopy methods. This approach allows us to identify multiple previously inaccessible excitons with wavefunctions residing in K, Γ, or Q valleys in the momentum space as well as various types of defect-related excitons. Overall, our approach is well-suited to unravel and tune intervalley excitons in various semiconductors.
arXiv: 2312.07332193. D. Schmitt, J. P. Bange, W. Bennecke, G. Meneghini, A. AlMutairi, M.Merboldt, J. Pöhls, K. Watanabe, T. Taniguchi, S. Steil, D. Steil, R. T. Weitz, S. Hofmann, S. Brem, G. S. Matthijs Jansen, E. Malic, S. Mathias and M. Reutzel "Ultrafast nano-imaging of dark excitons", arXiv: 2305.18908
The role and impact of spatial heterogeneity in two-dimensional quantum materials represents one of the major research quests regarding the future application of these materials in optoelectronics and quantum information science. In the case of transition-metal dichalcogenide heterostructures, in particular, direct access to heterogeneities in the dark-exciton landscape with nanometer spatial and ultrafast time resolution is highly desired, but remains largely elusive. Here, we introduce ultrafast dark field momentum microscopy to spatio-temporally resolve dark exciton formation dynamics in a twisted WSe2/MoS2 heterostructure with 55 femtosecond time- and 500~nm spatial resolution. This allows us to directly map spatial heterogeneity in the electronic and excitonic structure, and to correlate these with the dark exciton formation and relaxation dynamics. The benefits of simultaneous ultrafast nanoscale dark-field momentum microscopy and spectroscopy is groundbreaking for the present study, and opens the door to new types of experiments with unprecedented spectroscopic and spatiotemporal capabilities.
arXiv: 2305.18908192. Q. Lin, H. Fang, Y. Liu, Y. Zhang, M. Fischer, J. Li, J. Hagel, S. Brem, E. Malic, N. Stenger, Z. Sun, M. Wubs, S. Xiao, "A room-temperature moiré interlayer exciton laser" arXiv: 2302.01266
Moiré superlattices in van der Waals heterostructures offer highly tunable quantum systems with emergent electronic and excitonic properties such as superconductivity, topological edge states, and moiré-trapped excitons. Theoretical calculations predicted the existence of the moiré potential at elevated temperatures; however, its impact on the optical properties of interlayer excitons (IXs) at room temperature is lacking, and the benefits of the moiré effects for lasing applications remain unexplored. We report that the moiré potential in a molybdenum disulfide/tungsten diselenide (MoS2/WSe2) heterobilayer system can significantly enhance light emission, elongate the IX lifetime, and modulate the IX emission energy at room temperature. By integrating a moiré superlattice with a silicon topological nanocavity, we achieve ultra-low-threshold lasing at the technologically important telecommunication O-band thanks to the significant moiré modulation. Moreover, the high-quality topological nanocavities facilitate the highest spectral coherence of < 0.1 nm linewidth among all reported two-dimensional material-based laser systems. Our findings not only open a new avenue for studying correlated states at elevated temperatures, but also enable novel architectures for integrated on-chip photonics and optoelectronics.
arXiv: 2302.01266