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Abstract: Plasmonic structures have attracted much interest in science and engineering disciplines, exploring a myriad of potential applications owing to their strong light-matter interactions. Recently, the plasmonic concentration of energy in subwavelength volumes has been used to initiate chemical reactions, for instance by combining plasmonic materials with catalytic metals. In this work, we demonstrate that plasmonic nanoparticles of earth-abundant Mg can undergo galvanic replacement in a nonaqueous solvent to produce decorated structures. This method yields bimetallic architectures where partially oxidized 200–300 nm Mg nanoplates and nanorods support many smaller Au, Ag, Pd, or Fe nanoparticles, with potential for a stepwise process introducing multiple decoration compositions on a single Mg particle. We investigated this mechanism by electron-beam imaging and local composition mapping with energy-dispersive X-ray spectroscopy as well as, at the ensemble level, by inductively coupled plasma mass spectrometry. High-resolution scanning transmission electron microscopy further supported the bimetallic nature of the particles and provided details of the interface geometry, which includes a Mg oxide separation layer between Mg and the other metal. Depending on the composition of the metallic decorations, strong plasmonic optical signals characteristic of plasmon resonances were observed in the bulk with ultraviolet-visible spectrometry and at the single particle level with darkfield scattering. These novel bimetallic and multimetallic designs open up an exciting array of applications where one or multiple plasmonic structures could interact in the near-field of earth-abundant Mg and couple with catalytic nanoparticles for applications in sensing and plasmon-assisted catalysis.

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Abstract: Here we study the high-temperature formation and dynamics of large inversion domains (IDs) that form in monolayer MoS2 using atomic-resolution annular dark-field scanning transmission electron microscopy (ADF-STEM) with an in situ heating stage. We use temperatures above 700 °C to thermally activate rapid S vacancy migration and this leads to a formation mechanism of IDs that differs from the one at room temperature, where S vacancy migration is limited. We show that at high temperatures the formation of IDs occurs from intersected networks of long S vacancy line defects, whose strain fields are non-orthogonal and trigger large scale atomic reconstructions. Once formed, the IDs are influenced by the dynamic behaviour of nearby line defects and voids. With Mo and S atoms undergoing movement, the two types of ID grain boundaries can shift to allow further expansion of the ID area along the adjoining line defects. We reveal that IDs serve as metastable configurations between line defect rearrangements and eventual void formation under electron beam irradiation during heating. The formation of voids near to the IDs causes them to revert back to pristine lattice, which has the effect of restricting the ID domain size to a certain range (e.g. 3–5 nm in our observation) instead of continuously enlarging. This study provides insights into how the MoS2 IDs form and evolve at high temperature and can benefit the tailoring of electronic properties of two dimensional materials by structural manipulation.

Open Access

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Abstract: Electron ptychography has recently attracted considerable interest for high resolution phase-sensitive imaging. However, to date studies have been mainly limited to radiation resistant samples as the electron dose required to record a ptychographic dataset is too high for use with beam-sensitive materials. Here we report defocused electron ptychography using a fast, direct-counting detector to reconstruct the transmission function, which is in turn related to the electrostatic potential of a two-dimensional material at atomic resolution under various low dose conditions.

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Abstract: A brittle material under loading fails by the nucleation and propagation of a sharp crack. In monatomic crystals, such as silicon, the lattice geometries front to the crack-tip changes the way of propagation even with the same cleavage surface. In general, however, crystals have multiple kinds of atoms and how the deformation of each atom affects the failure is still elusive. Here, we show that local atomic distortions from the different types of atoms causes a propagation anisotropy in suspended WS2 monolayers by combining annular dark-field scanning transmission electron microscopy and empirical molecular dynamics that are validated by first-principles calculations. Conventional conditions for brittle failure such as surface energy, elasticity, and crack geometry cannot account for this anisotropy. Further simulations predict the enhancement of the strengths and fracture toughness of the materials by designing void shapes and edge structures.