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Robust optical emission polarization in MoS2 monolayers through selective valley excitation

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 Added by Bernhard Urbaszek
 Publication date 2012
  fields Physics
and research's language is English




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We report polarization resolved photoluminescence from monolayer MoS2, a two-dimensional, non-centrosymmetric crystal with direct energy gaps at two different valleys in momentum space. The inherent chiral optical selectivity allows exciting one of these valleys and close to 90% polarized emission at 4K is observed with 40% polarization remaining at 300K. The high polarization degree of the emission remains unchanged in transverse magnetic fields up to 9T indicating robust, selective valley excitation.



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We report experimental evidences on selective occupation of the degenerate valleys in MoS2 monolayers by circularly polarized optical pumping. Over 30% valley polarization has been observed at K and K valley via the polarization resolved luminescence spectra on pristine MoS2 monolayers. It demonstrates one viable way to generate and detect valley polarization towards the conceptual valleytronics applications with information carried by the valley index.
Monolayers of transition metal dichalcogenides (TMDCs) are atomically thin direct-gap semiconductors with potential applications in nanoelectronics, optoelectronics, and electrochemical sensing. Recent theoretical and experimental efforts suggest that they are ideal systems for exploiting the valley degrees of freedom of Bloch electrons. For example, Dirac valley polarization has been demonstrated in mechanically exfoliated monolayer MoS2 samples by polarization-resolved photoluminescence, although polarization has rarely been seen at room temperature. Here we report a new method for synthesizing high optical quality monolayer MoS2 single crystals up to 25 microns in size on a variety of standard insulating substrates (SiO2, sapphire and glass) using a catalyst-free vapor-solid growth mechanism. The technique is simple and reliable, and the optical quality of the crystals is extremely high, as demonstrated by the fact that the valley polarization approaches unity at 30 K and persists at 35% even at room temperature, suggesting a virtual absence of defects. This will allow greatly improved optoelectronic TMDC monolayer devices to be fabricated and studied routinely.
Various types of defects in MoS2 monolayers and their influence on the electronic structure and transport properties have been studied using the Density-Functional based Tight-Binding method in conjunction with the Greens Function approach. Intrinsic defects in MoS2 monolayers significantly affect their electronic properties. Even at low concentration they considerably alter the quantum conductance. While the electron transport is practically isotropic in pristine MoS2, strong anisotropy is observed in the presence of defects. Localized mid-gap states are observed in semiconducting MoS2 that do not contribute to the conductivity but direction-dependent scatter the current, and that the conductivity is strongly reduced across line defects and selected grain boundary models.
357 - C. Robert , M.A. Semina , F. Cadiz 2017
The optical properties of MoS2 monolayers are dominated by excitons, but for spectrally broad optical transitions in monolayers exfoliated directly onto SiO2 substrates detailed information on excited exciton states is inaccessible. Encapsulation in hexagonal boron nitride (hBN) allows approaching the homogenous exciton linewidth, but interferences in the van der Waals heterostructures make direct comparison between transitions in optical spectra with different oscillator strength more challenging. Here we reveal in reflectivity and in photoluminescence excitation spectroscopy the presence of excited states of the A-exciton in MoS2 monolayers encapsulated in hBN layers of calibrated thickness, allowing to extrapolate an exciton binding energy of about 220 meV. We theoretically reproduce the energy separations and oscillator strengths measured in reflectivity by combining the exciton resonances calculated for a screened two-dimensional Coulomb potential with transfer matrix calculations of the reflectivity for the van der Waals structure. Our analysis shows a very different evolution of the exciton oscillator strength with principal quantum number for the screened Coulomb potential as compared to the ideal two-dimensional hydrogen model.
Anomalous valley Hall (AVH) effect is a fundamental transport phenomenon in the field of condensed-matter physics. Usually, the research on AVH effect is mainly focused on 2D lattices with ferromagnetic order. Here, by means of model analysis, we present a general design principle for realizing AVH effect in antiferromagnetic monolayers, which involves the introduction of nonequilibrium potentials to break of PT symmetry. Using first-principles calculations, we further demonstrate this design principle by stacking antiferromagnetic monolayer MnPSe3 on ferroelectric monolayer Sc2CO2 and achieve the AVH effect. The AVH effect can be well controlled by modulating the stacking pattern. In addition, by reversing the ferroelectric polarization of Sc2CO2 via electric field, the AVH effect in monolayer MnPSe3 can be readily switched on or off. The underlying physics are revealed in detail. Our findings open up a new direction of research on exploring AVH effect.
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