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Electronic Hybridization of Large-Area Stacked Graphene Films

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 Added by Jeremy Robinson
 Publication date 2013
  fields Physics
and research's language is English




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Direct, tunable coupling between individually assembled graphene layers is a next step towards designer two-dimensional (2D) crystal systems, with relevance for fundamental studies and technological applications. Here we describe the fabrication and characterization of large-area (> cm^2), coupled bilayer graphene on SiO2/Si substrates. Stacking two graphene films leads to direct electronic interactions between layers, where the resulting film properties are determined by the local twist angle. Polycrystalline bilayer films have a stained-glass window appearance explained by the emergence of a narrow absorption band in the visible spectrum that depends on twist angle. Direct measurement of layer orientation via electron diffraction, together with Raman and optical spectroscopy, confirms the persistence of clean interfaces over large areas. Finally, we demonstrate that interlayer coupling can be reversibly turned off through chemical modification, enabling optical-based chemical detection schemes. Together, these results suggest that individual 2D crystals can be individually assembled to form electronically coupled systems suitable for large-scale applications.

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The observation of the electrically tunable and highly confined plasmons in graphene has stimulated the exploration of interesting properties of plasmons in other two dimensional materials. Recently, hyperbolic plasmon resonance modes are observed in exfoliated WTe2 films, a type-II Weyl semimetal with layered structure, providing a platform for the assembly of plasmons with hyperbolicity and exotic topological properties. However, the plasmon modes were observed in relatively thick and small-area films, which restrict the tunability and application for plasmons. Here, large-area (~ cm) WTe2 films with different thickness are grown by chemical vapor deposition method, in which plasmon resonance modes are observed in films with different thickness down to about 8 nm. Hybridization of plasmon and surface polar phonons of the substrate is revealed by mapping the plasmon dispersion. The plasmon frequency is demonstrated to be tunable by changing the temperature and film thickness. Our results facilitate the development of a tunable and scalable WTe2 plasmonic system for revealing topological properties and towards various applications in sensing, imaging and light modulation.
Scalable fabrication of magnetic 2D materials and heterostructures constitutes a crucial step for scaling down current spintronic devices and the development of novel spintronic applications. Here, we report on van der Waals (vdW) epitaxy of the layered magnetic metal Fe$_3$GeTe$_2$ - a 2D crystal with highly tunable properties and a high prospect for room temperature ferromagnetism - directly on graphene by employing molecular beam epitaxy. Morphological and structural characterization confirmed the realization of large-area, continuous Fe$_3$GeTe$_2$/graphene heterostructure films with stable interfaces and good crystalline quality. Furthermore, magneto-transport and X-ray magnetic circular dichroism investigations confirmed a robust out-of-plane ferromagnetism in the layers, comparable to state-of-the-art exfoliated flakes from bulk crystals. These results are highly relevant for further research on wafer-scale growth of vdW heterostructures combining Fe$_3$GeTe$_2$ with other layered crystals such as transition metal dichalcogenides for the realization of multifunctional, atomically thin devices.
We present flexible photodetectors (PDs) for visible wavelengths fabricated by stacking centimetre-scale chemical vapour deposited (CVD) single layer graphene (SLG) and single layer CVD MoS2, both wet transferred onto a flexible polyethylene terephthalate substrate. The operation mechanism relies on injection of photoexcited electrons from MoS2 to the SLG channel. The external responsivity is 45.5A/W and the internal 570A/W at 642nm. This is at least two orders of magnitude higher than bulk-semiconductor flexible membranes and other flexible PDs based on graphene and layered materials. The photoconductive gain is up to 4x10^5. The photocurrent is in the 0.1-100 uA range. The devices are semi-transparent, with just 8% absorption at 642nm and work stably upon bending to a curvature of 6cm. These capabilities and the low voltage operation (<1V) make them attractive for wearable applications.
Large-area bilayer graphene (BG) is grown epitaxially on Ru(0001) surface and characterized by low temperature scanning tunneling microscopy. The lattice of the bottom layer of BG is stretched by 1.2%, while strain is absent from the top layer. The lattice mismatch between the two layers leads to the formation of a moire pattern with a periodicity of ~21.5 nm and a mixture of AA- and AB-stacking. The root3 x root3 superstructure around atomic defects is attributed to the inter-valley scattering of the delocalized pi-electrons, demonstrating that the as-grown BG behaves like intrinsic free-standing graphene.
The synthesis of transition metal dichalcogenides (TMDs) has been a primary focus for 2D nanomaterial research over the last 10 years, however, only a small fraction of this research has been concentrated on transition metal ditellurides. In particular, nanoscale platinum ditelluride (PtTe2) has rarely been investigated, despite its potential applications in catalysis, photonics and spintronics. Of the reports published, the majority examine mechanically-exfoliated flakes from chemical vapor transport (CVT) grown crystals. While this production method is ideal for fundamental studies, it is very resource intensive therefore rendering this process unsuitable for large scale applications. In this report, the synthesis of thin films of PtTe2 through the reaction of solid-phase precursor films is described. This offers a production method for large-area, thickness-controlled PtTe2, suitable for a range of applications. These polycrystalline PtTe2 films were grown at temperatures as low as 450 degC, significantly below the typical temperatures used in the CVT synthesis methods. To investigate their potential applicability, these films were examined as electrocatalysts for the hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR). The films showed promising catalytic behavior, however, the PtTe2 was found to undergo chemical transformation to a substoichiometric chalcogenide compound under ORR conditions. This study shows while PtTe2 is stable and highly useful for HER, this property does not apply to ORR, which undergoes a fundamentally different mechanism. This study broadens our knowledge of the electrocatalysis of TMDs.
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