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Register a new userRydberg series of dark excitons and the conduction band spin-orbit splitting in monolayer WSe$_2$
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Added by
Piotr Kapu\\'sci\\'nski
Publication date
2021
fields
Physics
and research's language is
English
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Strong Coulomb correlations together with multi-valley electronic bands in the presence of spin-orbit interaction and possible new optoelectronic applications are at the heart of studies of the rich physics of excitons in semiconductor structures made of monolayers of transition metal dichalcogenides (TMD). In intrinsic TMD monolayers the basic, intravalley excitons are formed by a hole from the top of the valence band and an electron either from the lower or upper spin-orbit-split conduction band subbands: one of these excitons is optically active, the second one is dark, although possibly observed under special conditions. Here we demonstrate the s-series of Rydberg dark exciton states in monolayer WSe$_2$, which appears in addition to a conventional bright exciton series in photoluminescence spectra measured in high in-plane magnetic fields. The comparison of energy ladders of bright and dark Rydberg excitons is shown to be a method to experimentally evaluate one of the missing band parameters in TMD monolayers: the amplitude of the spin-orbit splitting of the conduction band.
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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.
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.
Charged excitons, or X$^{pm}$-trions, in monolayer transition metal dichalcogenides have binding energies of several tens of meV. Together with the neutral exciton X$^0$ they dominate the emission spectrum at low and elevated temperatures. We use charge tunable devices based on WSe$_2$ monolayers encapsulated in hexagonal boron nitride, to investigate the difference in binding energy between X$^+$ and X$^-$ and the X$^-$ fine structure. We find in the charge neutral regime, the X$^0$ emission accompanied at lower energy by a strong peak close to the longitudinal optical (LO) phonon energy. This peak is absent in reflectivity measurements, where only the X$^0$ and an excited state of the X$^0$ are visible. In the $n$-doped regime, we find a closer correspondence between emission and reflectivity as the trion transition with a well-resolved fine-structure splitting of 6~meV for X$^-$ is observed. We present a symmetry analysis of the different X$^+$ and X$^-$ trion states and results of the binding energy calculations. We compare the trion binding energy for the $n$-and $p$-doped regimes with our model calculations for low carrier concentrations. We demonstrate that the splitting between the X$^+$ and X$^-$ trions as well as the fine structure of the X$^-$ state can be related to the short-range Coulomb exchange interaction between the charge carriers.
Monolayer transition metal dichalcogenides are a promising platform to investigate many-body interactions of excitonic complexes. In monolayer tungsten diselenide, the ground-state exciton is dark (spin-indirect), and the valley degeneracy allows low-energy dark momentum-indirect excitons to form. Interactions between the dark exciton species and the optically accessible bright exciton (X) are likely to play significant roles in determining the optical properties of X at high power, as well as limiting the ultimate exciton densities that can be achieved, yet so far little is known about these interactions. Here, we demonstrate long-lived dense populations of momentum-indirect intervalley ($X_K$) and spin-indirect intravalley (D) dark excitons by time-resolved photoluminescence measurements (Tr-PL). Our results uncover an efficient inter-state conversion between X to D excitons through the spin-flip process and the one between D and $X_K$ excitons mediated by the exchange interaction (D + D to $X_K$ + $X_K$). Moreover, we observe a persistent redshift of the X exciton due to strong excitonic screening by $X_K$ exciton with a response time in the timescale of sub-ns, revealing a non-trivial inter-state exciton-exciton interaction. Our results provide a new insight into the interaction between bright and dark excitons, and point to a possibility to employ dark excitons for investigating exciton condensation and the valleytronics.
We present the electronic and structural properties of monolayer WSe$_{2}$ grown by pulsed-laser deposition on monolayer graphene (MLG) on SiC. The spin splitting in the WSe$_{2}$ valence band at $overline{mathrm{K}}$ was $Delta_mathrm{SO}=0.469pm0.008$ eV by angle-resolved photoemission spectroscopy (ARPES). Synchrotron-based grazing-incidence in-plane X-ray diffraction (XRD) revealed the in-plane lattice constant of monolayer WSe$_{2}$ to be $a_mathrm{WSe_2}=3.2757pm0.0008 mathrm{r{A}}$. This indicates a lattice compression of -0.19 % from bulk WSe$_{2}$. By using experimentally determined graphene lattice constant ($a_mathrm{MLG}=2.4575pm0.0007 mathrm{r{A}}$), we found that a 3$times$3 unit cell of the slightly compressed WSe$_{2}$ is perfectly commensurate with a 4$times$4 graphene lattice with a mismatch below 0.03 %, which could explain why the monolayer WSe$_{2}$ is compressed on MLG. From XRD and first-principles calculations, however, we conclude that the observed size of strain is negligibly small to account for a discrepancy in $Delta_mathrm{SO}$ found between exfoliated and epitaxial monolayers in earlier ARPES. In addition, angle-resolved, ultraviolet and X-ray photoelectron spectroscopy shed light on the band alignment between WSe$_{2}$ and MLG/SiC and indicate electron transfer from graphene to the WSe$_{2}$ monolayer. As further revealed by atomic force microscopy, the WSe$_{2}$ island size depends on the number of carbon layers on top of the SiC substrate. This suggests that the epitaxy of WSe$_{2}$ favors the weak van der Waals interactions with graphene while it is perturbed by the influence of the SiC substrate and its carbon buffer layer.
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