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Register a new userValley-selective chiral phonon replicas of dark excitons and trions in monolayer WSe2
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We observe a set of three replica luminescent peaks at ~21.4 meV below the dark exciton, negative and positive dark trions (or exciton-polarons) in monolayer WSe2. The replica redshift energy matches the energy of the zone-center E-mode optical phonons. The phonon replicas exhibit parallel gate dependence and same g-factors as the dark excitonic states, but follow the valley selection rules of the bright excitonic states. While the dark states exhibit out-of-plane transition dipole and valley-independent linearly polarized emission in the in-plane directions, their phonon replicas exhibit in-plane transition dipole and valley-dependent circularly polarized emission in the out-of-plane directions. Our results and symmetry analysis show that the K-valley dark exciton decays into a left-handed chiral phonon and a right-handed photon, whereas the K-valley dark exciton decays into a right-handed chiral phonon and a left-handed photon. Such valley selection rules of chiral phonon replicas can be utilized to identify the valleys of the dark excitonic states and explore their chiral interactions with phonons.
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Monolayer transition metal dichalcogenide (TMDC) crystals, as direct-gap materials with unusually strong light-matter interaction, have attracted much recent attention. In contrast to the initial understanding, the minima of the conduction band are predicted to be spin split. Because of this splitting and the spin-polarized character of the valence bands, the lowest-lying excitonic states in WX2 (X=S, Se) are expected to be spin-forbidden and optically dark. To date, however, there has been no direct experimental probe of these dark band-edge excitons, which strongly influence the light emission properties of the material. Here we show how an in-plane magnetic field can brighten the dark excitonic states and allow their properties to be revealed experimentally in monolayer WSe2. In particular, precise energy levels for both the neutral and charged dark excitons were obtained and compared with ab-initio calculations using the GW-BSE approach. Greatly increased emission and valley lifetimes were observed for the brightened dark states as a result of their spin configuration. These studies directly probe the excitonic spin manifold and provide a new route to tune the optical and valley properties of these prototypical two-dimensional semiconductors.
Single-layer transition metal dichalcogenides (TMDs) provide a promising material system to explore the electrons valley degree of freedom as a quantum information carrier. The valley degree of freedom in single-layer TMDs can be directly accessed by means of optical excitation. The rapid valley relaxation of optically excited electron-hole pairs (excitons) through the long-range electron-hole exchange interaction, however, has been a major roadblock. Theoretically such a valley relaxation does not occur for the recently discovered dark excitons, suggesting a potential route for long valley lifetimes. Here we investigate the valley dynamics of dark excitons in single-layer WSe2 by time-resolved photoluminescence spectroscopy. We develop a waveguide-based method to enable the detection of the dark exciton emission, which involves spin-forbidden optical transitions with an out-of-plane dipole moment. The valley degree of freedom of dark excitons is accessed through the valley-dependent Zeeman effect under an out-of-plane magnetic field. We find a short valley lifetime for the dark neutral exciton, likely due to the short-range electron-hole exchange, but long valley lifetimes exceeding several nanoseconds for dark charged excitons.
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 much insight into the internal quantum structure of trions and the complex excitonic interactions with defects and chiral phonons in monolayer valley semiconductors.
The presence of two spin-split valleys in monolayer (1L) transition metal dichalcogenide (TMD) semiconductors supports versatile exciton species classified by their spin and valley quantum numbers. While the spin-0 intravalley exciton, known as the bright exciton, is readily observable, other types of excitons, such as the spin-1 intravalley (spin-dark) and spin-0 intervalley (momentum-dark) excitons, are more difficult to access. Here we develop a waveguide coupled 1L tungsten diselenide (WSe2) device to probe these exciton species. In particular, TM coupling to the atomic layers out-of-plane dipole moments enabled us to not only efficiently collect, but also resonantly populate the spin-1 dark excitons, promising for developing devices with long valley lifetimes. Our work reveals several upconversion processes that bring out an intricate coupling network linking spin-0 and spin-1 intra- and inter-valley excitons, demonstrating that intervalley scattering and spin-flip are very common processes in the atomic layer. These experimental results deepen our understanding of tungsten diselenide exciton physics and illustrate that planar photonic devices are capable of harnessing versatile exciton species in TMD semiconductors.
Monolayers of semiconducting transition metal dichalcogenides are two-dimensional direct-gap systems which host tightly-bound excitons with an internal degree of freedom corresponding to the valley of the constituting carriers. Strong spin-orbit interaction and the resulting ordering of the spin-split subbands in the valence and conduction bands makes the lowest-lying excitons in WX$_2$ (X~being S or Se) spin-forbidden and optically dark. With polarization-resolved photoluminescence experiments performed on a WSe$_2$ monolayer encapsulated in a hexagonal boron nitride, we show how the intrinsic exchange interaction in combination with the applied in-plane and/or out-of-plane magnetic fields enables one to probe and manipulate the valley degree of freedom of the dark excitons.
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