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Tungsten-based monolayer transition metal dichalcogenides host a long-lived “dark” exciton, an electron-hole pair in a spin-triplet configuration. The long lifetime and unique spin properties of the dark exciton provide exciting opportunities to explore light-matter interactions beyond electric dipole transitions. Here we demonstrate that the coupling of the dark exciton and an optically silent chiral phonon enables the intrinsic photoluminescence of the dark-exciton replica in monolayer WSe 2 . Gate and magnetic-field dependent PL measurements unveil a circularly-polarized replica peak located below the dark exciton by 21.6 meV, equal to E″ phonon energy from Se vibrations. First-principles calculations show that the exciton-phonon interaction selectively couples the spin-forbidden dark exciton to the intravalley spin-allowed bright exciton, permitting the simultaneous emission of a chiral phonon and a circularly-polarized photon. Our discovery and understanding of the phonon replica reveals a chirality dictated emission channel of the phonons and photons, unveiling a new route of manipulating valley-spin. The long lifetime and spin properties of dark excitons in atomically thin transition metal dichalcogenides offer opportunities to explore light-matter interactions beyond electric dipole transitions. Here, the authors demonstrate that the coupling of the dark exciton and an optically silent chiral phonon enables the intrinsic photoluminescence of the dark-exciton replica in monolayer WSe 2

The heterostructure of monolayer transition metal dichalcogenides (TMDCs) provides a unique platform to manipulate exciton dynamics. The ultrafast carrier transfer across the van der Waals interface of the TMDC hetero-bilayer can efficiently separate electrons and holes in the intralayer excitons with a type II alignment, but it will funnel excitons into one layer with a type I alignment. In this work, we demonstrate the reversible switch from exciton dissociation to exciton funneling in a MoSe 2 /WS 2 heterostructure, which manifests itself as the photoluminescence (PL) quenching to PL enhancement transition. This transition was realized through effectively controlling the quantum capacitance of both MoSe 2 and WS 2 layers with gating. PL excitation spectroscopy study unveils that PL enhancement arises from the blockage of the optically excited electron transfer from MoSe 2 to WS 2 . Our work demonstrates electrical control of photoexcited carrier transfer across the van der Waals interface, the understanding of which promises applications in quantum optoelectronics. The ultrafast carrier dynamics across the van der Waals interface of transition metal dichalcogenide heterostructures govern the formation and funnelling of excitons. Here, the authors demonstrate a reversible switch from exciton dissociation to exciton funnelling in a MoSe 2 /WS 2 heterostructure, which manifests itself as a photoluminescence quenching-to-enhancement transition.

Strong Coulomb interactions in single-layer transition metal dichalcogenides (TMDs) result in the emergence of strongly bound excitons, trions, and biexcitons. These excitonic complexes possess the valley degree of freedom, which can be exploited for quantum optoelectronics. However, in contrast to the good understanding of the exciton and trion properties, the binding energy of the biexciton remains elusive, with theoretical calculations and experimental studies reporting discrepant results. In this work, we resolve the conflict by employing low-temperature photoluminescence spectroscopy to identify the biexciton state in BN-encapsulated single-layer WSe 2 . The biexciton state only exists in charge-neutral WSe 2 , which is realized through the control of efficient electrostatic gating. In the lightly electron-doped WSe 2 , one free electron binds to a biexciton and forms the trion–exciton complex. Improved understanding of the biexciton and trion–exciton complexes paves the way for exploiting the many-body physics in TMDs for novel optoelectronics applications. Owing to strong Coulomb interactions, atomically thin transition metal dichalcogenides host strongly bound excitonic complexes. Here, the authors report charge-neutral biexciton and negatively charged trion-exciton complexes in hBN encapsulated monolayer WSe 2 by employing low-temperature photoluminescence spectroscopy.

The enhanced Coulomb interaction in two dimensions leads to not only tightly bound excitons but also many-particle excitonic complexes: excitons interacting with other quasiparticles, which results in improved and even new exciton properties with better controls. Here, we summarize studies of excitonic complexes in monolayer transition metal dichalcogenides and their moiré heterojunctions, envisioning how to utilize them for exploring quantum many-body physics.

Transition metal dichalcogenide (TMDC) moiré superlattices, owing to the moiré flatbands and strong correlation, can host periodic electron crystals and fascinating correlated physics. The TMDC heterojunctions in the type-II alignment also enable long-lived interlayer excitons that are promising for correlated bosonic states, while the interaction is dictated by the asymmetry of the heterojunction. Here we demonstrate a new excitonic state, quadrupolar exciton, in a symmetric WSe 2 -WS 2 -WSe 2 trilayer moiré superlattice. The quadrupolar excitons exhibit a quadratic dependence on the electric field, distinctively different from the linear Stark shift of the dipolar excitons in heterobilayers. This quadrupolar exciton stems from the hybridization of WSe 2 valence moiré flatbands. The same mechanism also gives rise to an interlayer Mott insulator state, in which the two WSe 2 layers share one hole laterally confined in one moiré unit cell. In contrast, the hole occupation probability in each layer can be continuously tuned via an out-of-plane electric field, reaching 100% in the top or bottom WSe 2 under a large electric field, accompanying the transition from quadrupolar excitons to dipolar excitons. Our work demonstrates a trilayer moiré system as a new exciting playground for realizing novel correlated states and engineering quantum phase transitions. The authors observe the signatures of quadrupolar excitons in a WSe 2 -WS 2 -WSe 2 trilayer moiré superlattice, originating from the hybridization of the WSe 2 valence moiré flatbands. They further use electrostatic gating to reveal a hybridized interlayer Mott insulator state, with holes shared between the two WSe 2 layers but laterally confined in moiré superlattices.

Strong many-body interaction in two-dimensional transitional metal dichalcogenides provides a unique platform to study the interplay between different quasiparticles, such as prominent phonon replica emission and modified valley-selection rules. A large out-of-plane magnetic field is expected to modify the exciton-phonon interactions by quantizing excitons into discrete Landau levels, which is largely unexplored. Here, we observe the Landau levels originating from phonon-exciton complexes and directly probe exciton-phonon interaction under a quantizing magnetic field. Phonon-exciton interaction lifts the inter-Landau-level transition selection rules for dark trions, manifested by a distinctively different Landau fan pattern compared to bright trions. This allows us to experimentally extract the effective mass of both holes and electrons. The onset of Landau quantization coincides with a significant increase of the valley-Zeeman shift, suggesting strong many-body effects on the phonon-exciton interaction. Our work demonstrates monolayer WSe 2 as an intriguing playground to study phonon-exciton interactions and their interplay with charge, spin, and valley. An out-of-plane magnetic field is expected to strongly modify exciton-phonon interactions in atomically thin transitional metal dichalcogenides. Here, the authors show that the phonon-exciton interaction in monolayer WSe 2 lifts the inter-Landau-level transition selection rules for dark trions.

Moiré superlattices of semiconducting transition metal dichalcogenides enable unprecedented spatial control of electron wavefunctions, leading to emerging quantum states. The breaking of translational symmetry further introduces a new degree of freedom: high symmetry moiré sites of energy minima behaving as spatially separated quantum dots. We demonstrate the superposition between two moiré sites by constructing a trilayer WSe 2 /monolayer WS 2 moiré heterojunction. The two moiré sites in the first layer WSe 2 interfacing WS 2 allow the formation of two different interlayer excitons, with the hole residing in either moiré site of the first layer WSe 2 and the electron in the third layer WSe 2 . An electric field can drive the hybridization of either of the interlayer excitons with the intralayer excitons in the third WSe 2 layer, realizing the continuous tuning of interlayer exciton hopping between two moiré sites and a superposition of the two interlayer excitons, distinctively different from the natural trilayer WSe 2 . The moiré lattice of trilayer WSe 2 and monolayer WS 2 host interlayer excitons localized at different moiré sites. Using an electric field, the authors tune the superposition between two moiré sites via hybridization with intralayer excitons in WSe 2 .

Semiconducting transition metal dichalcogenide (TMDC) moiré superlattices provide an unprecedented platform for manipulating excitons. The in-situ control of moiré excitons could enable novel excitonic devices but remains challenging. Meanwhile, as dipolar composite bosons, interlayer excitons in the type-II aligned TMDC moiré superlattices exhibit strong interactions with fermionic charge carriers. Here, we demonstrate active manipulation of exciton diffusivity by tuning their interplay with correlated carriers in moiré potentials. When electrons form Mott insulators, the interlayer exciton energy is blueshifted due to strong electron-exciton repulsion, leading to the enhancement of diffusivity by as much as two orders of magnitude. In contrast, exciton diffusivity is suppressed at fractional fillings, where carriers form generalized Wigner crystals. In between fractional fillings, electrons populate all moiré traps, resulting in enhanced diffusivity with increasing carrier density, owing to the effectively reduced moiré potential confinement experienced by excitons. Our study inspires further engineering and controlling exotic excitonic states in TMDC moiré superlattices for fascinating quantum phenomena and novel excitonic devices. The study shows that exciton diffusivity in semiconducting moiré superlattices can be strongly modulated by correlated electrons, revealing intriguing interactions and ushering in avenues for quantum optoelectronic technologies.

Atomic defects are easily created in the single-layer electronic devices of current interest and cause even more severe influence than in the bulk devices since the electronic quantum paths are obviously suppressed in the two-dimensional transport. Here we find a drop of chemical solution can repair the defects in the single-layer MoSe 2 field-effect transistors. The devices’ room-temperature electronic mobility increases from 0.1 cm 2 /Vs to around 30 cm 2 /Vs and hole mobility over 10 cm 2 /Vs after the solution processing. The defect dynamics is interpreted by the combined study of the first-principles calculations, aberration-corrected transmission electron microscopy, and Raman spectroscopy. Rich single/double Selenium vacancies are identified by the high-resolution microscopy, which cause some mid-gap impurity states and localize the device carriers. They are found to be repaired by the processing with the result of extended electronic states. Such a picture is confirmed by a 1.5 cm −1 red shift in the Raman spectra. Two-dimensional materials: Repairing atomic defects via solution processing Defects can heavily influence the electrical transport properties of three-dimensional materials. But their impact becomes even more pronounced in low-dimensional systems. Fengqi Song and colleagues use a combination of calculations and experiments to show that a simple drop of a chemical solution can repair the selenium vacancies in field-effect transistors made from single layer molybdenum diselenide. By reducing the number of vacancies, which localize the electronic transport, the authors increased the carrier mobilities to nearly the intrinsic value by 2–3 orders of magnitude. The defect dynamics is visualized by the high resolution electron microscopy and multislice simulations. Such an approach could provide a route for enabling practical devices to be made from these relatively fragile materials.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.An amendment to this paper has been published and can be accessed via a link at the top of the paper.