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Identifying defect-related quantum emitters in monolayer WSe$_2$

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 Added by Xiulai Xu Prof
 Publication date 2020
  fields Physics
and research's language is English




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Monolayer transition metal dichalcogenides have recently attracted great interests because the quantum dots embedded in monolayer can serve as optically active single photon emitters. Here, we provide an interpretation of the recombination mechanisms of these quantum emitters through polarization-resolved and magneto-optical spectroscopy at low temperature. Three types of defect-related quantum emitters in monolayer tungsten diselenide (WSe$_2$) are observed, with different exciton g factors of 2.02, 9.36 and unobservable Zeeman shift, respectively. The various magnetic response of the spatially localized excitons strongly indicate that the radiative recombination stems from the different transitions between defect-induced energy levels, valance and conduction bands. Furthermore, the different g factors and zero-field splittings of the three types of emitters strongly show that quantum dots embedded in monolayer have various types of confining potentials for localized excitons, resulting in electron-hole exchange interaction with a range of values in the presence of anisotropy. Our work further sheds light on the recombination mechanisms of defect-related quantum emitters and paves a way toward understanding the role of defects in single photon emitters in atomically thin semiconductors.

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Quantum light sources in solid-state systems are of major interest as a basic ingredient for integrated quantum device technologies. The ability to tailor quantum emission through deterministic defect engineering is of growing importance for realizing scalable quantum architectures. However, a major difficulty is that defects need to be positioned site-selectively within the solid. Here, we overcome this challenge by controllably irradiating single-layer MoS$_{2}$ using a sub-nm focused helium ion beam to deterministically create defects. Subsequent encapsulation of the ion bombarded MoS$_{2}$ flake with high-quality hBN reveals spectrally narrow emission lines that produce photons at optical wavelengths in an energy window of one to two hundred meV below the neutral 2D exciton of MoS$_{2}$. Based on ab-initio calculations we interpret these emission lines as stemming from the recombination of highly localized electron-hole complexes at defect states generated by the helium ion bombardment. Our approach to deterministically write optically active defect states in a single transition metal dichalcogenide layer provides a platform for realizing exotic many-body systems, including coupled single-photon sources and exotic Hubbard systems.
Recent developments in fabrication of van der Waals heterostructures enable new type of devices assembled by stacking atomically thin layers of two-dimensional materials. Using this approach, we fabricate light-emitting devices based on a monolayer WSe$_2$, and also comprising boron nitride tunnelling barriers and graphene electrodes, and observe sharp luminescence spectra from individual defects in WSe$_2$ under both optical and electrical excitation. This paves the way towards the realization of electrically-pumped quantum emitters in atomically thin semiconductors. In addition we demonstrate tuning by more than 1 meV of the emission energy of the defect luminescence by applying a vertical electric field. This provides an estimate of the permanent electric dipole created by the corresponding electron-hole pair. The light-emitting devices investigated in our work can be assembled on a variety of substrates enabling a route to integration of electrically pumped single quantum emitters with existing technologies in nano-photonics and optoelectronics.
Monolayer (ML) semiconducting transition-metal dichalcogenides (TMDs) represent a unique class of two-dimensional (2D) electron systems. Their atomically thin structure -- just like graphene -- facilitates gate-tunability, while the sizable band gap and strong spin-orbit coupling hold promise for properties beyond graphene. Measurements under large magnetic fields have revealed an unusual LL structure, distinct from other 2D electron systems. However, owing to limited sample quality and poor electrical contact, probing the lowest Landau levels (LLs) has been challenging, and observation of electron correlations within the fractionally filled LLs regime has not been possible. Here, through bulk electronic compressibility measurements, we investigate the LL structure of ML WSe$_2$ in the extreme quantum limit, and observe fractional quantum Hall (FQH) states in the lowest three LLs. The odd-denominator FQH sequences demonstrate a systematic evolution with the LL orbital index, which has not been observed in any other system but is consistent with generic theoretical expectations. In addition, we observe an even-denominator state in the second LL that is expected to host non-Abelian statistics. Our results suggest that the 2D semiconductors can provide an experimental platform that closely resembles idealized theoretical models in the quantum Hall regime.
We report the fabrication and characterization of gate-defined hole quantum dots in monolayer and bilayer WSe$_2$. The devices were operated with gates above and below the WSe$_2$ layer to accumulate a hole gas, which for some devices was then selectively depleted to define the dot. Temperature dependence of conductance in the Coulomb blockade regime is consistent with transport through a single level, and excited state transport through the dots was observed at temperatures up to 10 K. For adjacent charge states of a bilayer WSe$_2$ dot, magnetic field dependence of excited state energies was used to estimate $g$-factors between 0.8 and 2.4 for different states. These devices provide a platform to evaluate valley-spin states in monolayer and bilayer WSe$_2$ for application as qubits.
248 - E. Courtade , M. Semina , M. Manca 2017
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.
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