Matching Items (5)

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Direct optical transitions at K- and H-point of Brillouin zone in bulk MoS2, MoSe2, WS2, and WSe2

Description

Modulated reflectance (contactless electroreflectance (CER), photoreflectance (PR), and piezoreflectance (PzR)) has been applied to study direct optical transitions in bulk MoS[subscript 2], MoSe[subscript 2], WS[subscript 2], and WSe[subscript 2]. In

Modulated reflectance (contactless electroreflectance (CER), photoreflectance (PR), and piezoreflectance (PzR)) has been applied to study direct optical transitions in bulk MoS[subscript 2], MoSe[subscript 2], WS[subscript 2], and WSe[subscript 2]. In order to interpret optical transitions observed in CER, PR, and PzR spectra, the electronic band structure for the four crystals has been calculated from the first principles within the density functional theory for various points of Brillouin zone including K and H points. It is clearly shown that the electronic band structure at H point of Brillouin zone is very symmetric and similar to the electronic band structure at K point, and therefore, direct optical transitions at H point should be expected in modulated reflectance spectra besides the direct optical transitions at the K point of Brillouin zone. This prediction is confirmed by experimental studies of the electronic band structure of MoS[subscript 2], MoSe[subscript 2], WS[subscript 2], and WSe[subscript 2] crystals by CER, PR, and PzR spectroscopy, i.e., techniques which are very sensitive to critical points of Brillouin zone. For the four crystals besides the A transition at K point, an A[subscript H] transition at H point has been observed in CER, PR, and PzR spectra a few tens of meV above the A transition. The spectral difference between A and A[subscript H] transition has been found to be in a very good agreement with theoretical predictions. The second transition at the H point of Brillouin zone (B[subscript H] transition) overlaps spectrally with the B transition at K point because of small energy differences in the valence (conduction) band positions at H and K points. Therefore, an extra resonance which could be related to the B[subscript H] transition is not resolved in modulated reflectance spectra at room temperature for the four crystals.

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Date Created
  • 2016-06-21

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Observation of ultralong valley lifetime in WSe2/MoS2 heterostructures

Description

The valley degree of freedom in two-dimensional (2D) crystals recently emerged as a novel information carrier in addition to spin and charge. The intrinsic valley lifetime in 2D transition metal

The valley degree of freedom in two-dimensional (2D) crystals recently emerged as a novel information carrier in addition to spin and charge. The intrinsic valley lifetime in 2D transition metal dichalcogenides (TMD) is expected to be markedly long due to the unique spin-valley locking behavior, where the intervalley scattering of the electron simultaneously requires a large momentum transfer to the opposite valley and a flip of the electron spin. However, the experimentally observed valley lifetime in 2D TMDs has been limited to tens of nanoseconds thus far. We report efficient generation of microsecond-long-lived valley polarization in WSe[subscript 2]/MoS[subscript 2] heterostructures by exploiting the ultrafast charge transfer processes in the heterostructure that efficiently creates resident holes in the WSe[subscript 2] layer. These valley-polarized holes exhibit near-unity valley polarization and ultralong valley lifetime: We observe a valley-polarized hole population lifetime of more than 1 μs and a valley depolarization lifetime (that is, intervalley scattering lifetime) of more than 40 μs at 10 K. The near-perfect generation of valley-polarized holes in TMD heterostructures, combined with ultralong valley lifetime, which is orders of magnitude longer than previous results, opens up new opportunities for novel valleytronics and spintronics applications.

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Created

Date Created
  • 2017-07-26

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Spin-orbit engineering in transition metal dichalcogenide alloy monolayers

Description

Binary transition metal dichalcogenide monolayers share common properties such as a direct optical bandgap, spin-orbit splittings of hundreds of meV, light–matter interaction dominated by robust excitons and coupled spin-valley states.

Binary transition metal dichalcogenide monolayers share common properties such as a direct optical bandgap, spin-orbit splittings of hundreds of meV, light–matter interaction dominated by robust excitons and coupled spin-valley states. Here we demonstrate spin-orbit-engineering in Mo[subscript (1−x)]W[subscript x]Se[subscript 2] alloy monolayers for optoelectronics and applications based on spin- and valley-control. We probe the impact of the tuning of the conduction band spin-orbit spin-splitting on the bright versus dark exciton population. For MoSe[subscript 2] monolayers, the photoluminescence intensity decreases as a function of temperature by an order of magnitude (4–300 K), whereas for WSe[subscript 2] we measure surprisingly an order of magnitude increase. The ternary material shows a trend between these two extreme behaviours. We also show a non-linear increase of the valley polarization as a function of tungsten concentration, where 40% tungsten incorporation is sufficient to achieve valley polarization as high as in binary WSe[subscript 2].

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Date Created
  • 2015-12-14

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Unusual lattice vibration characteristics in whiskers of the pseudo-one-dimensional titanium trisulfide TiS3

Description

Transition metal trichalcogenides form a class of layered materials with strong in-plane anisotropy. For example, titanium trisulfide (TiS[subscript 3]) whiskers are made out of weakly interacting TiS[subscript 3] layers, where

Transition metal trichalcogenides form a class of layered materials with strong in-plane anisotropy. For example, titanium trisulfide (TiS[subscript 3]) whiskers are made out of weakly interacting TiS[subscript 3] layers, where each layer is made of weakly interacting quasi-one-dimensional chains extending along the b axis. Here we establish the unusual vibrational properties of TiS[subscript 3] both experimentally and theoretically. Unlike other two-dimensional systems, the Raman active peaks of TiS[subscript 3] have only out-of-plane vibrational modes, and interestingly some of these vibrations involve unique rigid-chain vibrations and S–S molecular oscillations. High-pressure Raman studies further reveal that the A[subscript g][superscript S–S] S-S molecular mode has an unconventional negative pressure dependence, whereas other peaks stiffen as anticipated. Various vibrational modes are doubly degenerate at ambient pressure, but the degeneracy is lifted at high pressures. These results establish the unusual vibrational properties of TiS[subscript 3] with strong in-plane anisotropy, and may have relevance to understanding of vibrational properties in other anisotropic two-dimensional material systems.

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Date Created
  • 2016-09-22

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Unusual dimensionality effects and surface charge density in 2D Mg(OH)2

Description

We present two-dimensional Mg(OH)[subscript 2] sheets and their vertical heterojunctions with CVD-MoS[subscript 2] for the first time as flexible 2D insulators with anomalous lattice vibration and chemical and physical properties.

We present two-dimensional Mg(OH)[subscript 2] sheets and their vertical heterojunctions with CVD-MoS[subscript 2] for the first time as flexible 2D insulators with anomalous lattice vibration and chemical and physical properties. New hydrothermal crystal growth technique enabled isolation of environmentally stable monolayer Mg(OH)[subscript 2] sheets. Raman spectroscopy and vibrational calculations reveal that the lattice vibrations of Mg(OH)[subscript 2] have fundamentally different signature peaks and dimensionality effects compared to other 2D material systems known to date. Sub-wavelength electron energy-loss spectroscopy measurements and theoretical calculations show that Mg(OH)[subscript 2] is a 6 eV direct-gap insulator in 2D, and its optical band gap displays strong band renormalization effects from monolayer to bulk, marking the first experimental confirmation of confinement effects in 2D insulators. Interestingly, 2D-Mg(OH)[subscript 2] sheets possess rather strong surface polarization (charge) effects which is in contrast to electrically neutral h-BN materials. Using 2D-Mg(OH)[subscript 2] sheets together with CVD-MoS[subscript 2] in the vertical stacking shows that a strong change transfer occurs from n-doped CVD-MoS[subscript 2] sheets to Mg(OH)[subscript 2], naturally depleting the semiconductor, pushing towards intrinsic doping limit and enhancing overall optical performance of 2D semiconductors. Results not only establish unusual confinement effects in 2D-Mg(OH)[subscript 2], but also offer novel 2D-insulating material with unique physical, vibrational, and chemical properties for potential applications in flexible optoelectronics.

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Created

Date Created
  • 2016-02-05