Signatures of moiré trions in WSe2/MoSe2 heterobilayers.

Moiré superlattices formed by van der Waals materials can support a wide range of electronic phases, including Mott insulators1-4, superconductors5-10 and generalized Wigner crystals2. When excitons are confined by a moiré superlattice, a new class of exciton emerges, which holds promise for realizing artificial excitonic crystals and quantum optical effects11-16. When such moiré excitons are coupled to charge carriers, correlated states may arise. However, no experimental evidence exists for charge-coupled moiré exciton states, nor have their properties been predicted by theory. Here we report the optical signatures of trions coupled to the moiré potential in tungsten diselenide/molybdenum diselenide heterobilayers. The moiré trions show multiple sharp emission lines with a complex charge-density dependence, in stark contrast to the behaviour of conventional trions. We infer distinct contributions to the trion emission from radiative decay in which the remaining carrier resides in different moiré minibands. Variation of the trion features is observed in different devices and sample areas, indicating high sensitivity to sample inhomogeneity and variability. The observation of these trion features motivates further theoretical and experimental studies of higher-order electron correlation effects in moiré superlattices.

Electrically Switchable Intervalley Excitons with Strong Two-Phonon Scattering in Bilayer WSe2.

We report the observation of QΓ intervalley exciton in bilayer WSe2 devices encapsulated by boron nitride. The QΓ exciton resides at ∼18 meV below the QK exciton. The QΓ and QK excitons exhibit different Stark shifts under an out-of-plane electric field due to their different interlayer dipole moments. By controlling the electric field, we can switch their energy ordering and control which exciton dominates the luminescence of bilayer WSe2. Remarkably, both QΓ and QK excitons exhibit unusually strong two-phonon replicas, which are comparable to or even stronger than the one-phonon replicas. By detailed theoretical simulation, we reveal the existence of numerous (≥14) two-phonon scattering paths involving (nearly) resonant exciton-phonon scattering in bilayer WSe2. To our knowledge, such electric-field-switchable intervalley excitons with strong two-phonon replicas have not been found in any other two-dimensional semiconductors. These make bilayer WSe2 a distinctive valleytronic material with potential novel applications.

Landau-Quantized Excitonic Absorption and Luminescence in a Monolayer Valley Semiconductor.

We investigate Landau-quantized excitonic absorption and luminescence of monolayer WSe_{2} under magnetic field. We observe gate-dependent quantum oscillations in the bright exciton and trions (or exciton polarons) as well as the dark trions and their phonon replicas. Our results reveal spin- and valley-polarized Landau levels (LLs) with filling factors n=+0, +1 in the bottom conduction band and n=-0 to -6 in the top valence band, including the Berry-curvature-induced n=±0 LLs of massive Dirac fermions. The LL filling produces periodic plateaus in the exciton energy shift accompanied by sharp oscillations in the exciton absorption width and magnitude. This peculiar exciton behavior can be simulated by semiempirical calculations. The experimentally deduced g factors of the conduction band (g∼2.5) and valence band (g∼15) exceed those predicted in a single-particle model (g=1.5, 5.5, respectively). Such g-factor enhancement implies strong many-body interactions in gated monolayer WSe_{2}. The complex interplay between Landau quantization, excitonic effects, and many-body interactions makes monolayer WSe_{2} a promising platform to explore novel correlated quantum phenomena.

Multipath Optical Recombination of Intervalley Dark Excitons and Trions in Monolayer WSe_{2}.

Excitons and trions (or exciton polarons) in transition metal dichalcogenides (TMDs) are known to decay predominantly through intravalley transitions. Electron-hole recombination across different valleys can also play a significant role in the excitonic dynamics, but intervalley transitions are rarely observed in monolayer TMDs, because they violate the conservation of momentum. Here we reveal the intervalley recombination of dark excitons and trions through more than one path in monolayer WSe_{2}. We observe the intervalley dark excitons, which can recombine by the assistance of defect scattering or chiral-phonon emission. We also reveal that a trion can decay in two distinct paths-through intravalley or intervalley electron-hole recombination-into two different final valley states. Although these two paths are energy degenerate, we can distinguish them by lifting the valley degeneracy under a magnetic field. In addition, the intra- and inter-valley trion transitions are coupled to zone-center and zone-corner chiral phonons, respectively, to produce distinct phonon replicas. The observed multipath optical decays of dark excitons and trions provide insight into the internal quantum structure of trions and the complex excitonic interactions with defects and chiral phonons in monolayer valley semiconductors.

Gate Tunable Dark Trions in Monolayer WSe_{2}.

Monolayer WSe_{2} is an intriguing material to explore dark exciton physics. We have measured the photoluminescence from dark excitons and trions in ultraclean monolayer WSe_{2} devices encapsulated by boron nitride. The dark trions can be tuned continuously between negative and positive trions with electrostatic gating. We reveal their spin-triplet configuration and distinct valley optical emission by their characteristic Zeeman splitting under a magnetic field. The dark trion binding energies are 14-16 meV, slightly lower than the bright trion binding energies (21-35 meV). The dark trion lifetime (∼1.3 ns) is two orders of magnitude longer than the bright trion lifetime (∼10 ps) and can be tuned between 0.4 and 1.3 ns by gating. Such robust, optically detectable, and gate tunable dark trions may help us realize trion transport in two-dimensional materials.

Exciton-polaron Rydberg states in monolayer MoSe2 and WSe2.

Exciton polaron is a hypothetical many-body quasiparticle that involves an exciton dressed with a polarized electron-hole cloud in the Fermi sea. It has been evoked to explain the excitonic spectra of charged monolayer transition metal dichalcogenides, but the studies were limited to the ground state. Here we measure the reflection and photoluminescence of monolayer MoSe2 and WSe2 gating devices encapsulated by boron nitride. We observe gate-tunable exciton polarons associated with the 1 s-3 s exciton Rydberg states. The ground and excited exciton polarons exhibit comparable energy redshift (15~30 meV) from their respective bare excitons. The robust excited states contradict the trion picture because the trions are expected to dissociate in the excited states. When the Fermi sea expands, we observe increasingly severe suppression and steep energy shift from low to high exciton-polaron Rydberg states. Their gate-dependent energy shifts go beyond the trion description but match our exciton-polaron theory. Our experiment and theory demonstrate the exciton-polaron nature of both the ground and excited excitonic states in charged monolayer MoSe2 and WSe2.