The strong light-matter interaction and the valley selective optical selection rules make monolayer (ML) MoS 2 an exciting 2D material for fundamental physics and optoelectronics applications. But, so far, optical transition linewidths even at low temperature are typically as large as a few tens of meV and contain homogeneous and inhomogeneous contributions. This prevented in-depth studies, in contrast to the bettercharacterized ML materials MoSe 2 and WSe 2 . In this work, we show that encapsulation of ML MoS 2 in hexagonal boron nitride can efficiently suppress the inhomogeneous contribution to the exciton linewidth, as we measure in photoluminescence and reflectivity a FWHM down to 2 meV at T ¼ 4 K. Narrow optical transition linewidths are also observed in encapsulated WS 2 , WSe 2 , and MoSe 2 MLs. This indicates that surface protection and substrate flatness are key ingredients for obtaining stable, high-quality samples. Among the new possibilities offered by the well-defined optical transitions, we measure the homogeneous broadening induced by the interaction with phonons in temperature-dependent experiments. We uncover new information on spin and valley physics and present the rotation of valley coherence in applied magnetic fields perpendicular to the ML.
We have investigated the exciton dynamics in transition metal
The optical selection rules for interband transitions in WSe_{2}, WS_{2}, and MoSe_{2} transition metal dichalcogenide monolayers are investigated by polarization-resolved photoluminescence experiments with a signal collection from the sample edge. These measurements reveal a strong polarization dependence of the emission lines. We see clear signatures of the emitted light with the electric field oriented perpendicular to the monolayer plane, corresponding to an interband optical transition forbidden at normal incidence used in standard optical spectroscopy measurements. The experimental results are in agreement with the optical selection rules deduced from group theory analysis, highlighting the key role played by the different symmetries of the conduction and valence bands split by the spin-orbit interaction. These studies yield a direct determination of the bright-dark exciton splitting, for which we measure 40±1 meV and 55±2 meV in WSe_{2} and WS_{2} monolayer, respectively.
Charged excitons, or X ± -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 WSe2 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. arXiv:1705.02110v2 [cond-mat.mes-hall] 9 May 2018
The intricate interplay between optically dark and bright excitons governs the light-matter interaction in transition metal dichalcogenide monolayers. We have performed a detailed investigation of the "spin-forbidden" dark excitons in WSe2 monolayers by optical spectroscopy in an out-of-plane magnetic field Bz. In agreement with the theoretical predictions deduced from group theory analysis, magneto-photoluminescence experiments reveal a zero field splitting δ=0.6 ± 0.1 meV between two dark exciton states. The low energy state being strictly dipole forbidden (perfectly dark) at Bz=0 while the upper state is partially coupled to light with z polarization («grey» exciton). The first determination of the dark neutral exciton lifetime τ D in a transition metal dichalcogenide monolayer is obtained by time-resolved photoluminescence. We measure τ D~1 10 ± 10 ps for the grey exciton state, i.e. two orders of magnitude longer than the radiative lifetime of the bright neutral exciton at T=12 K.
Excitons, Coulomb bound electron–hole pairs, are composite bosons and their interactions in traditional semiconductors lead to condensation and light amplification. The much stronger Coulomb interaction in transition metal dichalcogenides such as WSe2 monolayers combined with the presence of the valley degree of freedom is expected to provide new opportunities for controlling excitonic effects. But so far the bosonic character of exciton scattering processes remains largely unexplored in these two-dimensional materials. Here we show that scattering between B-excitons and A-excitons preferably happens within the same valley in momentum space. This leads to power dependent, negative polarization of the hot B-exciton emission. We use a selective upconversion technique for efficient generation of B-excitons in the presence of resonantly excited A-excitons at lower energy; we also observe the excited A-excitons state 2s. Detuning of the continuous wave, low-power laser excitation outside the A-exciton resonance (with a full width at half maximum of 4 meV) results in vanishing upconversion signal.
The direct gap interband transitions in transition metal dichalcogenide monolayers are governed by chiral optical selection rules. Determined by laser helicity, optical transitions in either the K^{+} or K^{-} valley in momentum space are induced. Linearly polarized laser excitation prepares a coherent superposition of valley states. Here, we demonstrate the control of the exciton valley coherence in monolayer WSe_{2} by tuning the applied magnetic field perpendicular to the monolayer plane. We show rotation of this coherent superposition of valley states by angles as large as 30° in applied fields up to 9 T. This exciton valley coherence control on the ps time scale could be an important step towards complete control of qubits based on the valley degree of freedom.
We have combined spatially-resolved steady-state micro-photoluminescence (µPL) with timeresolved photoluminescence (TRPL) to investigate the exciton diffusion in a WSe2 monolayer encapsulated with hexagonal boron nitride (hBN). At 300 K, we extract an exciton diffusion length LX = 0.36 ± 0.02 µm and an exciton diffusion coefficient of DX = 14.5 ± 2 cm 2 /s. This represents a nearly 10-fold increase in the effective mobility of excitons with respect to several previously reported values on nonencapsulated samples. At cryogenic temperatures, the high optical quality of these samples has allowed us to discriminate the diffusion of the different exciton species : bright and dark neutral excitons, as well as charged excitons. The longer lifetime of dark neutral excitons yields a larger diffusion length of L X D = 1.5 ± 0.02 µm.Introduction.-Two-dimensional crystals of transition metal dichalcogenides (TMDC) such as MX 2 (M=Mo, W; X=S, Se, Te) are promising atomically flat semiconductors for applications in nanoelectronics and optoelectronics [1][2][3][4][5]. For example, solar cells [6],photodetectors [7] and laser prototypes [8] based on mono or few-layer MoS 2 have been recently demonstrated. In addition to their potential for unconventional, atomically thin and flexible optoelectronics, the interplay between inversion symmetry breaking and strong spin-orbit coupling in monolayers (MLs) also yields unique spin/valley properties which are expected to provide additional functionalities in future devices [9][10][11][12][13][14][15].
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