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      Quantum plasmonic hot electron injection in the lateral heterostructure of WSe2-MoSe2

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          Abstract

          Lateral two-dimensional (2D) transitional metal dichalcogenide (TMD) heterostructures have recently attracted a wide attention as promising materials for optoelectronic nano-devices. Due to the nanometer-size width of the lateral heterojunction, the study of its photoemission properties is challenging and requires using subwavelength optical techniques. We investigated the photoresponse of a lateral 2D WSe2-MoSe2 heterostructure using tip-enhanced photoluminescence (TEPL) with sub-nanometer scale variable tip-sample distance. The controllable gold-coated plasmonic silver tip allows for both optical nano-imaging and plasmon-induced hot electron injection into the heterostructure, mediated by the depletion region between the MoSe2 and WSe2. This directionality contributes to the unequal enhancement of the TEPL signals from the MoSe2 and WSe2 sides of the heterojunction. By adjusting the tip-sample distance, we demonstrated the controllability of the hot electron injection rate. In particular, when the tip-sample distance reached the sub-nanometer van der Waals separation, the quantum plasmonic effects facilitated the hot electron injection. The properties of the directional hot electron injection in the quantum plasmonic regime make the lateral 2D MoSe2-WSe2 heterostructures promising for quantum nano-devices with tunable photoresponse.

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          Van der Waals heterostructures

          Research on graphene and other two-dimensional atomic crystals is intense and likely to remain one of the hottest topics in condensed matter physics and materials science for many years. Looking beyond this field, isolated atomic planes can also be reassembled into designer heterostructures made layer by layer in a precisely chosen sequence. The first - already remarkably complex - such heterostructures (referred to as 'van der Waals') have recently been fabricated and investigated revealing unusual properties and new phenomena. Here we review this emerging research area and attempt to identify future directions. With steady improvement in fabrication techniques, van der Waals heterostructures promise a new gold rush, rather than a graphene aftershock.
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            Plasmon-induced hot-electron generation at nanoparticle/metal-oxide interfaces for photovoltaic and photocatalytic devices

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              Chemical mapping of a single molecule by plasmon-enhanced Raman scattering.

              Visualizing individual molecules with chemical recognition is a longstanding target in catalysis, molecular nanotechnology and biotechnology. Molecular vibrations provide a valuable 'fingerprint' for such identification. Vibrational spectroscopy based on tip-enhanced Raman scattering allows us to access the spectral signals of molecular species very efficiently via the strong localized plasmonic fields produced at the tip apex. However, the best spatial resolution of the tip-enhanced Raman scattering imaging is still limited to 3-15 nanometres, which is not adequate for resolving a single molecule chemically. Here we demonstrate Raman spectral imaging with spatial resolution below one nanometre, resolving the inner structure and surface configuration of a single molecule. This is achieved by spectrally matching the resonance of the nanocavity plasmon to the molecular vibronic transitions, particularly the downward transition responsible for the emission of Raman photons. This matching is made possible by the extremely precise tuning capability provided by scanning tunnelling microscopy. Experimental evidence suggests that the highly confined and broadband nature of the nanocavity plasmon field in the tunnelling gap is essential for ultrahigh-resolution imaging through the generation of an efficient double-resonance enhancement for both Raman excitation and Raman emission. Our technique not only allows for chemical imaging at the single-molecule level, but also offers a new way to study the optical processes and photochemistry of a single molecule.
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                Author and article information

                Journal
                07 December 2017
                Article
                1712.02715
                d9de66df-13e9-443f-9f61-ede014a43f40

                http://arxiv.org/licenses/nonexclusive-distrib/1.0/

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                physics.optics physics.app-ph

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