Patterning of transition metal dichalcogenides catalyzed by surface plasmons with atomic precision

•The etching of two-dimensional TMDs is driven by planar SPPs•Desired layers are achieved tuning the light power and incident direction•Strong plasmonic coupling at Au/MoS2 interface induces oxidation dissolution Plasmonic metal/transition metal dichalcogenide (TMD) heterostructures have attracted a considerable interest owing to plasmon-induced interfacial charge transfer, which has emerged as an important topic in photocatalysis photovoltaics. In this work, we found exotic interaction with surface plasmon polaritons, can be exploited general method fabricate controllable lateral sizes. Taking MoS2 example, strong accumulate holes valence band weaken its interlayer interaction. Meanwhile, hot electrons would transfer on produce oxidizing H2O2 etch top layer aqueous media. By controlling power, monolayer, bilayer, trilayer pristine size. Our findings offer deep insights into metal-TMDs interfaces, opening up new avenue for controlled fabrication TMDs. 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Gao Tao Plasmonic-based electrochemical impedance electrical activities cells.Angew. 56: 8855-8859Crossref (42) Through matching, red wavelength 660 nm irradiated certain angle, i.e., resonant angle (Figure S1). resulting electromagnetic oscillating propagated Au/water interface, evanescent field penetration depth approximately 200 nm. employed bifunctional setup triggering monitoring layer-controlled 1). typical procedure, multilayered nanoflakes bulk crystals transferred them onto gold-coated glass coverslip S2). Surprisingly, observed phenomenon under deionized (DI) water. Optical images nanoflake before after 40 min clearly show morphological changes when red-light (1.7 mW·mm−2) (Figures 2A 2B ). video process, presented Video S1, reveals gradually etched away increasing time. Finally, thinner same experiment remained substrate. Because beam diameter (ca. 0.9 mm) far beyond propagation length ca. 6.5 μm, expected within etched. https://www.cell.com/cms/asset/0fd08fc8-9779-49d6-8317-066d4fa425bc/mmc2.mp4Loading ... Download .mp4 (0.52 MB) Help files S1. movie showing process quantify remaining substrate, measured thickness force microscopy (AFM). height residual 2.6 2C), corresponds MoS2. also Raman spectroscopy characterize etching. spectrum sensitive number, reading out frequency difference 20, 22, 23 cm−1 nanoflakes, respectively.37Lee Yan Brus L.E. Heinz Hone Ryu Anomalous lattice vibrations single- few-layer MoS2.ACS 4: 2695-2700Crossref (3445) spectra exhibit two characteristic vibrational modes, E2g1 (in-plane) A1g 2D), respectively. shows obvious smaller 23.1 between peaks than (24.9 cm−1), suggesting identified three MoS2, consistent abovementioned AFM analysis. further increased precisely regulated bilayer monolayer. When 3.4 mW·mm−2, more transparent 2E 2F). After etching, ~1.83 corresponded 2G). This identification corroborated 21.4 2H). continued increase 6.8 preserved substrate 2I 2J). Both 0.87 20.2 validated structure 2K 2L). More examples trilayer, SPPs-driven (SPPE) displayed similar differences (see details Figure S3), implying robust Notably, retain flakes, feasible other mechanical-force-driven bottom-up growth methods, providing meet demands fabrication. assumed underlying our work originated role SPPs. verify hypothesis, conducted experiments demonstrate responsible nanoflakes. First, changed p-polarized s-polarized recorded unaffected S4A–S4C). films, commonly excites much efficiently light, larger amplitude normal electric field.38Wang Seideman Petek Dynamics coupled polariton wave packets subwavelength slit optically thin films.Phys. 86: 165408Crossref (21) Second, illuminated vertically without excitation unchanged S4D–S4F). Third, exclude irradiation bare indium tin oxide-coated slide total internal reflection configuration S4G–S4L). 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Consequently, accumulation facilitates Different classic mechanical peeled away, case interlayer-expanded removed dissolution. introduced, suppressed, although repulsion exist. does prevent coupling, prohibits O2, latter limits electrons. suggest repulsion, electrons, decay, processes together contribute overall layer. adjacent stem affinity sulfur bond strength.52Häkkinen gold-sulfur nanoscale.Nat. 443-455Crossref (1191) Density theory (DFT) calculations binding value 1.43 J/m2 confirming S12). applied materials, including WS2, MoSe2, ternary MoS2xSe2(1−x) S13), showed features. interestingly, direction, easily tuned changing position path. direction-dependent behavior S2. Figures 4B 4D several snapshots left right, occurred side extended center direction 4A 4B). adjusted right left, edge began central region 4C 4D). whole https://www.cell.com/cms/asset/2d2fc88b-8b9b-4445-90b8-6ef8b9568e85/mmc3.mp4Loading (2.13 reveal anisotropic behavior, captured scattering pattern 4E). encountering higher contrast COMSOL Multiphysics software simulate S14). simulated distribution nanoflake, decreasing 4F). strongest images. offset S15), conformed above results. simulation spatial determines Based capability here, proof-of-concept patterning manipulating duration 5A). 5B homostructure obtained domain switching initiation SPP, designed homostructures selection shape, size, domains explicitly patterned 5C), possibilities realizing novel MoS2-based electronic devices. area diameter, enlarge large-scale setups, prism SPPE versatile, being applicable artificial architectures, techniques. processing nanoscale manipulation utilized future micro-/nanoprocessing technology. summary, successfully tuneable materials. Thick monolayers, trilayers varying output while preserving combination calculations, revealed production ROS weakened exited event, diverse deeper photochemistry plasmon-matter interactions, offering paradigm physical