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Register a new userThe interplay between excitons and trions in a monolayer of MoSe$_2$
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Evgenia Cherotchenko
Publication date
2017
fields
Physics
and research's language is
English
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We study the impact of a free carrier reservoir on the optical properties of excitonic and trionic complexes in a MoSe$_2$ monolayer at cryogenic temperatures. By applying photodoping via a non-resonant pump laser the electron density can be controlled in our sample and in turn the exciton and trion densities can be tuned. We find a significant increase of the trion binding energy in the presence of an induced electron gas both in power- and in time-resolved photoluminescence spectra. This behaviour is reproduced within the original variational approach that takes into account both screening and phase space filling effects.
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Interfacing atomically thin van der Waals semiconductors with magnetic substrates enables additional control on their intrinsic valley degree of freedom and provides a promising platform for the development of novel valleytronic devices for information processing and storage. Here we study circularly polarized photoluminescence in heterostructures of monolayer MoSe$_2$ and thin films of ferrimagnetic bismuth iron garnet. We observe strong emission from charged excitons with negative valley polarization, which switches sign with increasing temperature, and demonstrate contrasting response to left and right circularly polarized excitation, associated with finite out-of-plane magnetization in the substrate. We propose a theoretical model accounting for magnetization-induced imbalance of charge carriers in the two valleys of MoSe$_2$, as well as for valley-switching scattering from B to A excitons and fast formation of trions with extended valley relaxation times, which shows excellent agreement with the experimental data. Our results provide new insights into valley physics in 2D semiconductors interfaced with magnetic substrates.
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.
Neutral and charged excitons (trions) in atomically-thin materials offer important capabilities for photonics, from ultrafast photodetectors to highly-efficient light-emitting diodes and lasers. Recent studies of van der Waals (vdW) heterostructures comprised of dissimilar monolayer materials have uncovered a wealth of optical phenomena that are predominantly governed by interlayer interactions. Here, we examine the optical properties in NbSe$_2$ - MoSe$_2$ vdW heterostructures, which provide an important model system to study metal-semiconductor interfaces, a common element in optoelectronics. Through low-temperature photoluminescence (PL) microscopy we discover a sharp emission feature, L1, that is localized at the NbSe$_2$-capped regions of MoSe$_2$. L1 is observed at energies below the commonly-studied MoSe$_2$ excitons and trions, and exhibits temperature- and power-dependent PL consistent with exciton localization in a confining potential. Remarkably, L1 is very robust not just in different samples, but also under a variety of fabrication processes. Using first-principles calculations we reveal that the confinement potential required for exciton localization naturally arises from the in-plane band bending due to the changes in the electron affinity between pristine MoSe$_2$ and NbSe$_2$ - MoSe$_2$ heterostructure. We discuss the implications of our studies for atomically-thin optoelectronics devices with atomically-sharp interfaces and tunable electronic structures.
Transition metal dichalcogenide heterobilayers offer attractive opportunities to realize lattices of interacting bosons with several degrees of freedom. Such heterobilayers can feature moire patterns that modulate their electronic band structure, leading to spatial confinement of single interlayer excitons (IXs) that act as quantum emitters with $C_3$ symmetry. However, the narrow emission linewidths of the quantum emitters contrast with a broad ensemble IX emission observed in nominally identical heterobilayers, opening a debate regarding the origin of IX emission. Here we report the continuous evolution from a few trapped IXs to an ensemble of IXs with both triplet and singlet spin configurations in a gate-tunable $2H$-MoSe$_2$/WSe$_2$ heterobilayer. We observe signatures of dipolar interactions in the IX ensemble regime which, when combined with magneto-optical spectroscopy, reveal that the narrow quantum-dot-like and broad ensemble emission originate from IXs trapped in moire potentials with the same atomic registry. Finally, electron doping leads to the formation of three different species of localised negative trions with contrasting spin-valley configurations, among which we observe both intervalley and intravalley IX trions with spin-triplet optical transitions. Our results identify the origin of IX emission in MoSe$_2$/WSe$_2$ heterobilayers and highlight the important role of exciton-exciton interactions and Fermi-level control in these highly tunable quantum materials.
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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