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Preprints
185. C. Chandrakant Palekar, J. Hagel, B. Rosa, S. Brem, C.- W. Shih, I. Limame, M. von Helversen, S. Tongay, E. Malic, S. Reitzenstein, "Twist Angle Dependence of Exciton Resonances in WSe2/MoSe2 Moiré Heterostructures", arXiv: 2309.16822
Van der Waals heterostructures based on TMDC semiconducting materials have emerged as promising materials due to their spin-valley properties efficiently contrived by the stacking-twist angle. The twist angle drastically alters the interlayer excitonic response by determining the spatial modulation, confining moiré potential, and atomic reconstruction in those systems. Nonetheless, the impact of the interlayer twist angle on the band alignment of the monolayers composing the heterostructure has received scant attention in the current research. Here, we systematically investigate the twist-angle dependence of intra- and interlayer excitons in twisted WSe2/MoSe2 heterobilayers. By performing photoluminescence excitation spectroscopy, we identify the twist-angle dependence of interlayer emission response, where an energy redshift of about 100 meV was observed for increasing twist angles. The applied microscopic theory predicts, on the contrary, a blueshift, which suggests that additional features, such as atomic reconstruction, may also surpass the moiré potential confinement. Those findings also prompt the effects of dielectric screening by addressing the redshift response to the stacking layer order. Furthermore, our findings support the evidence of a band offset dependence on the twist angle for the adjacent monolayers composing the heterobilayer system. Our fundamental study of exciton resonances deepens the current understanding of the physics of twisted TMDC heterostructures and paves the way for future experiments and theoretical works.
arXiv: 2309.16822184. J. Hagel, S. Brem, J. Abelardo Pineiro, E. Malic, "Impact of atomic reconstruction on optical spectra of twisted TMD homobilayers", arXiv: 2308.14633
Twisted bilayers of transition metal dichalcogenides (TMDs) have revealed a rich exciton landscape including hybrid excitons and spatially trapped moiré excitons that dominate the optical response of the material. Recent studies have revealed that in the low-twist-angle regime, the lattice undergoes a significant relaxation in order to minimize local stacking energies. Here, large domains of low energy stacking configurations emerge, deforming the crystal lattices via strain and consequently impacting the electronic band structure. However, so far the direct impact of atomic reconstruction on the exciton energy landscape and the optical properties has not been well understood. Here, we apply a microscopic and material-specific approach and predict a significant change in the potential depth for moiré excitons in a reconstructed lattice, with the most drastic change occurring in TMD homobilayers. We reveal the appearance of multiple flat bands and a significant change in the position of trapping sites compared to the rigid lattice. Most importantly, we predict a multi-peak structure emerging in optical absorption of WSe2 homobilayers - in stark contrast to the single peak that dominates the rigid lattice. This finding can be exploited as an unambiguous signature of atomic reconstruction in optical spectra of moiré excitons in twisted homobilayers.
arXiv: 2308.14633183. H. Fang, Q. Lin, Y. Zhang, J. Thompson, S. Xiao, Z. Sun, E. Malic, S. Dash, W. Wieczorek, "Localization and interaction of interlayer excitons in MoSe2/WSe2 heterobilayers", arXiv: 2307.03842
Transition metal dichalcogenide (TMD) heterobilayers provide a versatile platform to explore unique excitonic physics via properties of the constituent TMDs and external stimuli. Interlayer excitons (IXs) can form in TMD heterobilayers as delocalized or localized states. However, the localization of IX in different types of potential traps, the emergence of biexcitons in the high-excitation regime, and the impact of potential traps on biexciton formation have remained elusive. In our work, we observe two types of potential traps in a MoSe2/WSe2 heterobilayer, which result in significantly different emission behavior of IXs at different temperatures. We identify the origin of these traps as localized defect states and the moir{é} potential of the TMD heterobilayer. Furthermore, with strong excitation intensity, a superlinear emission behavior indicates the emergence of interlayer biexcitons, whose formation peaks at a specific temperature. Our work elucidates the different excitation and temperature regimes required for the formation of both localized and delocalized IX and biexcitons, and, thus, contributes to a better understanding and application of the rich exciton physics in TMD heterostructures.
arXiv: 2307.03842182. R. Perea-Causin, S. Brem, O. Schmidt, E. Malic "Trion photoluminescence and trion stability in atomically thin semiconductors", arXiv: 2306.10812
The optical response of doped monolayer semiconductors is governed by trions, i.e. photoexcited electron-hole pairs bound to doping charges. While their photoluminescence (PL) signatures have been identified in experiments, a microscopic model consistently capturing bright and dark trion peaks is still lacking. In this work, we derive a generalized trion PL formula on a quantum-mechanical footing, considering direct and phonon-assisted recombination mechanisms. We show the trion energy landscape in WSe2 by solving the trion Schrödinger equation. We reveal that the mass imbalance between equal charges results in less stable trions exhibiting a small binding energy and, interestingly, a large energetic offset from exciton peaks in PL spectra. Furthermore, we compute the temperature-dependent PL spectra for n- and p-doped monolayers and predict yet unobserved signatures originating from trions with an electron at the Λ point. Our work presents an important step towards a microscopic understanding of the internal structure of trions determining their stability and optical fingerprint.
arXiv: 2306.10812181. 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: 2305.18908180. J. P. Bange, D. Schmitt, W. Bennecke , G. Meneghini, A. AlMutairi, K. Watanabe, T. Taniguchi, D. Steil, S. Steil, R. T. Weitz, G. S. M. Jansen, S. Hofmann, S. Brem, E. Malic, M. Reutzel, S. Mathias "Probing correlations in the exciton landscape of a moiré heterostructure", arXiv: 2303.17886
Excitons are two-particle correlated bound states that are formed due to Coulomb interaction between single-particle holes and electrons. In the solid-state, cooperative interactions with surrounding quasiparticles can strongly tailor the exciton properties and potentially even create new correlated states of matter. It is thus highly desirable to access such cooperative and correlated exciton behavior on a fundamental level. Here, we find that the ultrafast transfer of an exciton's hole across a type-II band-aligned moiré heterostructure leads to a surprising sub-200-fs upshift of the single-particle energy of the electron being photoemitted from the two-particle exciton state. While energy relaxation usually leads to an energetic downshift of the spectroscopic signature, we show that this unusual upshift is a clear fingerprint of the correlated interactions of the electron and hole parts of the exciton quasiparticle. In this way, time-resolved photoelectron spectroscopy is straightforwardly established as a powerful method to access exciton correlations and cooperative behavior in two-dimensional quantum materials. Our work highlights this new capability and motivates the future study of optically inaccessible correlated excitonic and electronic states in moiré heterostructures.
arXiv: 2303.17886179. 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: 2302.01266178. C. Linderälv, J. Hagel, S. Brem, E. Malic, P. Erhart, "The moiré potential in twisted transition metal dichalcogenide bilayers", arXiv: 2205.15616
Moiré superlattices serve as a playground for emerging phenomena, such as localization of band states, superconductivity, and localization of excitons. These superlattices are large and are often modeled in the zero-angle limit, which obscures the effect of finite twist angles. Here, by means of first-principles calculations we quantify the twist-angle dependence of the moiré potential in the MoS homobilayer and identify the contributions from the constituent elements of the moiré potential. Furthermore, by considering the zero-angle limit configurations, we show that the moiré potential is rather homogeneous across the transition metal dichalcogenides (TMDs) and briefly discuss the separate effects of potential shifts and hybridization on the bilayer hybrid excitons. We find that the moiré potential in TMDs exhibits both an electrostatic component and a hybridization component, which are intertwined and have different relative strengths in different parts of the Brillouin zone. The electrostatic component of the moiré potential is a varying dipole field, which has a strong twist angle dependence. In some cases, the hybridization component can be interpreted as a tunneling rate but the interpretation is not generally applicable over the full Brillouin zone.
arXiv: 2205.15616