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Abstract Moiré superlattices in van der Waals heterostructures represent a highly tunable quantum system, attracting substantial interest in both many-body physics and device applications. However, the influence of the moiré potential on light-matter interactions at room temperature has remained largely unexplored. In our study, we demonstrate that the moiré potential in MoS2/WSe2 heterobilayers facilitates the localization of interlayer exciton (IX) at room temperature. By performing reflection contrast spectroscopy, we demonstrate the importance of atomic reconstruction in modifying intralayer excitons, supported by the atomic force microscopy experiment. When decreasing the twist angle, we observe that the IX lifetime becomes longer and light emission gets enhanced, indicating that non-radiative decay channels such as defects are suppressed by the moiré potential. Moreover, through the integration of moiré superlattices with silicon single-mode cavities, we find that the devices employing moiré-trapped IXs exhibit a significantly lower threshold, one order of magnitude smaller compared to the device utilizing delocalized IXs. These findings not only encourage the exploration of many-body physics in moiré superlattices at elevated temperatures but also pave the way for leveraging these artificial quantum materials in photonic and optoelectronic applications.

Abstract Doped van der Waals heterostructures host layer-hybridized trions, i.e. charged excitons with layer-delocalized constituents holding promise for highly controllable optoelectronics. Combining a microscopic theory with photoluminescence (PL) experiments, we demonstrate the electrical tunability of the trion energy landscape in naturally stacked WSe2 bilayers. We show that an out-of-plane electric field modifies the energetic ordering of the lowest lying trion states, which consist of layer-hybridized $$\Lambda$$ Λ -point electrons and layer-localized K-point holes. At small fields, intralayer-like trions yield distinct PL signatures in opposite doping regimes characterized by weak Stark shifts in both cases. Above a doping-asymmetric critical field, interlayer-like species are energetically favored and produce PL peaks with a pronounced Stark red-shift and a counter-intuitively large intensity arising from efficient phonon-assisted recombination. Our work presents an important step forward in the microscopic understanding of layer-hybridized trions in van der Waals heterostructures and paves the way towards optoelectronic applications based on electrically controllable atomically-thin semiconductors.

Abstract Intervalley excitons with electron and hole wavefunctions residing in different valleys determine the long-range transport and dynamics observed in many semiconductors. However, these excitons with vanishing oscillator strength do not directly couple to light and, hence, remain largely unstudied. Here, we develop a simple nanomechanical technique to control the energy hierarchy of valleys via their contrasting response to mechanical strain. We use our technique to discover previously inaccessible intervalley excitons associated with K, Γ, or Q valleys in prototypical 2D semiconductors WSe2 and WS2. We also demonstrate a new brightening mechanism, rendering an otherwise “dark” intervalley exciton visible via strain-controlled hybridization with an intravalley exciton. Moreover, we classify various localized excitons from their distinct strain response and achieve large tuning of their energy. Overall, our valley engineering approach establishes a new way to identify intervalley excitons and control their interactions in a diverse class of 2D systems.

Abstract Transition metal dichalcogenide (TMD) heterobilayers provide a versatile platform to explore unique excitonic physics via the 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 moiré 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.

Abstract We report the emergence of dark-excitons in transition-metal-dichalcogenide (TMD) heterostructures that strongly rely on the stacking sequence, i.e., momentum-dark K-Q exciton located exclusively at the top layer of the heterostructure. The feature stems from band renormalization and is distinct from those of typical neutral excitons or trions, regardless of materials, substrates, and even homogeneous bilayers, which is further confirmed by scanning tunneling spectroscopy. To understand the unusual stacking sequence, we introduce the excitonic Elliot formula by imposing strain exclusively on the top layer that could be a consequence of the stacking process. We further find that the intensity ratio of Q- to K-excitons in the same layer is inversely proportional to laser power, unlike for conventional K-K excitons. This can be a metric for engineering the intensity of dark K-Q excitons in TMD heterostructures, which could be useful for optical power switches in solar panels.

Atomically thin semiconductors have been in the center of one of the most active research fields. Here, we discuss the main challenges in exciton transport that is crucial for nanoelectronics. We focus on transport phenomena in monolayers, lateral heterostructures, and twisted heterostacks of transition metal dichalcogenides.

Abstract The existence of bound charge transfer (CT) excitons at the interface of monolayer lateral heterojunctions has been debated in literature, but contrary to the case of interlayer excitons in vertical heterostructure their observation still has to be confirmed. Here, we present a microscopic study investigating signatures of bound CT excitons in photoluminescence spectra at the interface of hBN-encapsulated lateral MoSe2-WSe2 heterostructures. Based on a fully microscopic and material-specific theory, we reveal the many-particle processes behind the formation of CT excitons and how they can be tuned via interface- and dielectric engineering. For junction widths smaller than the Coulomb-induced Bohr radius we predict the appearance of a low-energy CT exciton. The theoretical prediction is compared with experimental low-temperature photoluminescence measurements showing emission in the bound CT excitons energy range. We show that for hBN-encapsulated heterostructures, CT excitons exhibit small binding energies of just a few tens meV and at the same time large dipole moments, making them promising materials for optoelectronic applications (benefiting from an efficient exciton dissociation and fast dipole-driven exciton propagation). Our joint theory-experiment study presents a significant step towards a microscopic understanding of optical properties of technologically promising 2D lateral heterostructures.

Strain engineering can manipulate the propagation of excitons in atomically thin transition metal dichalcogenides. Here, the authors observe an anti-funnelling behavior, i.e., the exciton photoluminescence moves away from high-strain regions, and attribute it to the dominating role of propagating dark excitons.

Here, the authors demonstrate proximity-controlled strong-coupling between Coulomb correlations and lattice dynamics in neighbouring van der Waals materials (WSe2 and a gypsum layer), creating electrically neutral hybrid exciton-phonon eigenmodes called excitonic Lyman polarons.

The crystallographic orientation of monolayers in van der Waals multi-layers controls their electronic and optical properties. Here the authors show how the twist angle affects Coulomb correlations governing the internal structure and the mutual interaction of excitons in homobilayers of WSe2.

The electronic band structure of atomically thin transition metal dichalcogenides is strongly sensitive to the number of layers, resulting in modified light emission. Here, the authors investigate the cryogenic emission from bilayer WSe2 to identify the role of momentum-indirect excitons for its optical response.

In atomically thin transition metal dichalcogenides, spin- and valley-polarised states can be addressed thanks to large spin–orbit coupling and circular dichroism. Here, the authors investigate theoretically and experimentally the decay dynamics of spin and valley polarisation in transition metal dichalcogenide monolayers.

Saturable absorption, a technologically relevant property of graphene, is usually explained with Pauli blocking of optically driven carriers in the strong-excitation regime. Here, Winzeret al. reveal a new saturation regime at low excitations, resulting in a double-bended saturation behaviour.

Two-dimensional materials have shown great promise as efficient chemical sensors. Here, the authors present a sensing mechanism to allow the detection of molecules based on dark excitons in atomically thin transition metal dichalcogenides.

The interplay between dark and bright excitons has a significant impact on the optical properties of semiconducting transition metal dichalcogenides. Here, the authors perform computational and experimental studies which unveil the microscopic origin of the excitonic coherence lifetime in WS2 and MoSe2.

Design of high-speed graphene-based devices relies on understanding of its ultrafast carrier dynamics. Here, the authors combine time-resolved terahertz spectroscopy and microscopic modelling to unveil the interplay between the scattering mechanisms dominating the ultrafast relaxation pathways in graphene.