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      High Q Hybrid Mie–Plasmonic Resonances in van der Waals Nanoantennas on Gold Substrate

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          Abstract

          Dielectric nanoresonators have been shown to circumvent the heavy optical losses associated with plasmonic devices; however, they suffer from less confined resonances. By constructing a hybrid system of both dielectric and metallic materials, one can retain low losses, while achieving stronger mode confinement. Here, we use a high refractive index multilayer transition-metal dichalcogenide WS 2 exfoliated on gold to fabricate and optically characterize a hybrid nanoantenna-on-gold system. We experimentally observe a hybridization of Mie resonances, Fabry–Perot modes, and surface plasmon-polaritons launched from the nanoantennas into the substrate. We measure the experimental quality factors of hybridized Mie–plasmonic (MP) modes to be up to 33 times that of standard Mie resonances in the nanoantennas on silica. We then tune the nanoantenna geometries to observe signatures of a supercavity mode with a further increased Q factor of over 260 in experiment. We show that this quasi-bound state in the continuum results from strong coupling between a Mie resonance and Fabry–Perot-plasmonic mode in the vicinity of the higher-order anapole condition. We further simulate WS 2 nanoantennas on gold with a 5 nm thick hBN spacer in between. By placing a dipole within this spacer, we calculate the overall light extraction enhancement of over 10 7, resulting from the strong, subwavelength confinement of the incident light, a Purcell factor of over 700, and high directivity of the emitted light of up to 50%. We thus show that multilayer TMDs can be used to realize simple-to-fabricate, hybrid dielectric-on-metal nanophotonic devices granting access to high- Q, strongly confined, MP resonances, along with a large enhancement for emitters in the TMD–gold gap.

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          Two-dimensional atomic crystals

          We report free-standing atomic crystals that are strictly 2D and can be viewed as individual atomic planes pulled out of bulk crystals or as unrolled single-wall nanotubes. By using micromechanical cleavage, we have prepared and studied a variety of 2D crystals including single layers of boron nitride, graphite, several dichalcogenides, and complex oxides. These atomically thin sheets (essentially gigantic 2D molecules unprotected from the immediate environment) are stable under ambient conditions, exhibit high crystal quality, and are continuous on a macroscopic scale.
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            Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides

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              Ultrafast charge transfer in atomically thin MoS₂/WS₂ heterostructures.

              Van der Waals heterostructures have recently emerged as a new class of materials, where quantum coupling between stacked atomically thin two-dimensional 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 two-dimensional 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 photoexcited MoS2/WS2 heterostructures using both photoluminescence mapping and femtosecond 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 two-dimensional layers. Such ultrafast charge transfer in van der Waals heterostructures can enable novel two-dimensional devices for optoelectronics and light harvesting.
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                Author and article information

                Journal
                ACS Nano
                ACS Nano
                nn
                ancac3
                ACS Nano
                American Chemical Society
                1936-0851
                1936-086X
                13 June 2024
                25 June 2024
                : 18
                : 25
                : 16208-16221
                Affiliations
                []Department of Physics and Astronomy, University of Sheffield , Sheffield S3 7RH, U.K.
                []Department of Physics, School of Physics, Engineering and Technology, University of York , York YO10 5DD, U.K.
                Author notes
                Author information
                https://orcid.org/0000-0001-7993-8218
                https://orcid.org/0000-0002-8414-4081
                https://orcid.org/0000-0001-8603-3468
                https://orcid.org/0000-0002-2482-005X
                https://orcid.org/0000-0002-4169-5510
                Article
                10.1021/acsnano.4c02178
                11210342
                38869002
                8348b354-e3c5-4ec4-9db5-c376ee3f845c
                © 2024 The Authors. Published by American Chemical Society

                Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained ( https://creativecommons.org/licenses/by/4.0/).

                History
                : 15 February 2024
                : 05 June 2024
                : 28 May 2024
                Funding
                Funded by: UK Research and Innovation, doi 10.13039/100014013;
                Award ID: EP/X02153X/1
                Funded by: Royal Academy of Engineering, doi 10.13039/501100000287;
                Award ID: RF/201718/17131
                Funded by: Engineering and Physical Sciences Research Council, doi 10.13039/501100000266;
                Award ID: EP/V026496/1
                Funded by: Engineering and Physical Sciences Research Council, doi 10.13039/501100000266;
                Award ID: EP/V007696/1
                Funded by: Engineering and Physical Sciences Research Council, doi 10.13039/501100000266;
                Award ID: EP/V006975/1
                Funded by: Engineering and Physical Sciences Research Council, doi 10.13039/501100000266;
                Award ID: EP/S030751/1
                Funded by: Graphene Flagship, doi 10.13039/100017697;
                Award ID: 881603
                Categories
                Article
                Custom metadata
                nn4c02178
                nn4c02178

                Nanotechnology
                van der waals materials,transition-metal dichalcogenides,nanophotonics,mie–plasmonic resonances,strong coupling,bound state in the continuum,purcell enhancement

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