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Register a new userScalable single-photon sources in atomically thin MoS2
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Real-world quantum applications, eg. on-chip quantum networks and quantum cryptography, necessitate large scale integrated single-photon sources with nanoscale footprint for modern information technology. While on-demand and high fidelity implantation of atomic scale single-photon sources in conventional 3D materials suffer from uncertainties due to the crystals dimensionality, layered 2D materials can host point-like centers with inherent confinement to a sub-nm plane. However, previous attempts to truly deterministically control spatial position and spectral homogeneity while maintaining the 2D character have not been realized. Here, we demonstrate the on-demand creation and precise positioning of single-photon sources in atomically thin MoS2 with very narrow ensemble broadening and near-unity fabrication yield. Focused ion beam irradiation creates 100s to 1000s of mono-typical atomistic defects with anti-bunched emission lines with sub-10 nm lateral and 0.7 nm axial positioning accuracy. Our results firmly establish 2D materials as a scalable platform for single-photon emitters with unprecedented control of position as well as photophysical properties owing to the all-interfacial nature.
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Atomically thin MoS$_{2}$ crystals have been recognized as a quasi-2D semiconductor with remarkable physics properties. This letter reports our Raman scattering measurements on multilayer and monolayer MoS$_{2}$, especially in the low-frequency range ($<$50 cm$^{-1}$). We find two low-frequency Raman modes with contrasting thickness dependence. With increasing the number of MoS$_{2}$ layers, one shows a significant increase in frequency while the other decreases following a 1/N (N denotes layer-number) trend. With the aid of first-principle calculations we assign the former as the shear mode $E_{2g}^{2}$ and the latter as the compression vibrational mode. The opposite evolution of the two modes with thickness demonstrates novel vibrational modes in atomically thin crystal as well as a new and more precise way to characterize thickness of atomically thin MoS$_{2}$ films. In addition, we observe a broad feature around 38 cm$^{-1}$ (~5 meV) which is visible only under near-resonance excitation and pinned at the fixed energy independent of thickness. We interpret the feature as an electronic Raman scattering associated with the spin-orbit coupling induced splitting in conduction band at K points in their Brillouin zone.
Electrons hopping in two-dimensional honeycomb lattices possess a valley degree of freedom in addition to charge and spin. In the absence of inversion symmetry, these systems were predicted to exhibit opposite Hall effects for electrons from different valleys. Such valley Hall effects have been achieved only by extrinsic means, such as substrate coupling, dual gating, and light illuminating. Here, we report the first observation of intrinsic valley Hall transport without any extrinsic symmetry breaking in the non-centrosymmetric monolayer and trilayer MoS2, evidenced by considerable nonlocal resistance that scales cubically with local resistance. Such a hallmark survives even at room temperature with a valley diffusion length at micron scale. By contrast, no valley Hall signal is observed in the centrosymmetric bilayer MoS2. Our work elucidates the topological quantum origin of valley Hall effects and marks a significant step towards the purely electrical control of valley degree of freedom in topological valleytronics.
Quantum emitters (QEs) in two-dimensional transition metal dichalcogenides (2D TMDCs) have advanced to the forefront of quantum communication and transduction research due to their unique potentials in accessing valley pseudo-spin degree of freedom (DOF) and facile integration into quantum-photonic, electronic and sensing platforms via the layer-by-layer-assembly approach. To date, QEs capable of operating in O-C telecommunication bands have not been demonstrated in TMDCs. Here we report a deterministic creation of such telecom QEs emitting over the 1080 to 1550 nm wavelength range via coupling of 2D molybdenum ditelluride (MoTe2) to strain inducing nano-pillar arrays. Our Hanbury Brown and Twiss experiment conducted at 10 K reveals clear photon antibunching with 90% single photon purity. Ultra-long lifetimes, 4-6 orders of magnitude longer than that of the 2D exciton, are also observed. Polarization analysis further reveals that while some QEs display cross-linearly polarized doublets with ~1 meV splitting resulting from the strain induced anisotropic exchange interaction, valley degeneracy is preserved in other QEs. Valley Zeeman splitting as well as restoring of valley symmetry in cross-polarized doublets are observed under 8T magnetic field. In contrast to other telecom QEs, our QEs which offer the potential to access valley DOF through single photons, could lead to unprecedented advantages in optical fiber-based quantum networks.
Raman scattering and photoluminescence spectroscopy are used to investigate the optical properties of single layer black phosphorus obtained by mechanical exfoliation of bulk crystals under an argon atmosphere. The Raman spectroscopy, performed in situ on the same flake as the photoluminescence measurements, demonstrates the single layer character of the investigated samples. The emission spectra, dominated by excitonic effects, display the expected in plane anisotropy. The emission energy depends on the type of substrate on which the flake is placed due to the different dielectric screening. Finally, the blue shift of the emission with increasing temperature is well described using a two oscillator model for the temperature dependence of the band gap.
Van der Waals heterostructures have recently emerged as a new class of materials, where quantum coupling between stacked atomically thin two-dimensional (2D) layers, including graphene, hexagonal-boron nitride, and transition metal dichalcogenides (MX2), give rise to fascinating new phenomena. MX2 heterostructures are particularly exciting for novel optoelectronic and photovoltaic applications, because 2D MX2 monolayers can have an optical bandgap in the near-infrared to visible spectral range and exhibit extremely strong light-matter interactions. Theory predicts that many stacked MX2 heterostructures form type-II semiconductor heterojunctions that facilitate efficient electron-hole separation for light detection and harvesting. Here we report the first experimental observation of ultrafast charge transfer in photo-excited MoS2/WS2 heterostructures using both photoluminescence mapping and femtosecond (fs) pump-probe spectroscopy. We show that hole transfer from the MoS2 layer to the WS2 layer takes place within 50 fs after optical excitation, a remarkable rate for van der Waals coupled 2D layers. Such ultrafast charge transfer in van der Waals heterostructures can enable novel 2D devices for optoelectronics and light harvesting.
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