5 research outputs found

    An [Fe<sup>III</sup><sub>30</sub>] molecular metal oxide

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    Dearle AE, Cutler DJ, Coletta M, et al. An [FeIII30] molecular metal oxide. Chemical Communications. 2021.Dissolution of FeBr3 in a mixture of acetonitrile and 3,4-lutidine in the presence of an amine results in the formation of an [Fe30] molecular metal oxide containing alternating layers of tetrahedral and octahedral FeIII ions. Mass spectrometry suggests the cluster is formed quickly and remains stable in solution, while magnetic measurements and DFT calculations reveal competing antiferromagnetic exchange interactions

    Imaging Light-Induced Migration of Dislocations in Halide Perovskites with 3D Nanoscale Strain Mapping

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    In recent years, halide perovskite materials have been used to make high performance solar cell and light-emitting devices. However, material defects still limit device performance and stability. Here, we use synchrotron-based Bragg Coherent Diffraction Imaging to visualise nanoscale strain fields, such as those local to defects, in halide perovskite microcrystals. We find significant strain heterogeneity within MAPbBr3_{3} (MA = CH3_{3}NH3+_{3}^{+}) crystals in spite of their high optoelectronic quality, and identify both ⟨\langle100⟩\rangle and ⟨\langle110⟩\rangle edge dislocations through analysis of their local strain fields. By imaging these defects and strain fields in situ under continuous illumination, we uncover dramatic light-induced dislocation migration across hundreds of nanometres. Further, by selectively studying crystals that are damaged by the X-ray beam, we correlate large dislocation densities and increased nanoscale strains with material degradation and substantially altered optoelectronic properties assessed using photoluminescence microscopy measurements. Our results demonstrate the dynamic nature of extended defects and strain in halide perovskites and their direct impact on device performance and operational stability.Comment: Main text and Supplementary Information. Main text: 15 pages, 4 figures. Supplementary Information: 16 pages, 27 figures, 1 tabl

    Understanding metal organic chemical vapour deposition of monolayer WS2: the enhancing role of Au substrate for simple organosulfur precursors.

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    We find that the use of Au substrate allows fast, self-limited WS2 monolayer growth using a simple sequential exposure pattern of low cost, low toxicity precursors, namely tungsten hexacarbonyl and dimethylsulfide (DMS). We use this model reaction system to fingerprint the technologically important metal organic chemical vapour deposition process by operando X-ray photoelectron spectroscopy (XPS) to address the current lack of understanding of the underlying fundamental growth mechanisms for WS2 and related transition metal dichalcogenides. Au effectively promotes the sulfidation of W with simple organosulfides, enabling WS2 growth with low DMS pressure (<1 mbar) and a suppression of carbon contamination of as-grown WS2, which to date has been a major challenge with this precursor chemistry. Full WS2 coverage can be achieved by one exposure cycle of 10 minutes at 700 °C. We discuss our findings in the wider context of previous literature on heterogeneous catalysis, 2D crystal growth, and overlapping process technologies such as atomic layer deposition (ALD) and direct metal conversion, linking to future integrated manufacturing processes for transition metal dichalcogenide layers.We acknowledge funding from EPSRC (EP/T001038/1, EP/P005152/1). V.-P.V.-R. acknowledges EPSRC Doctoral Training Award (EP/M508007/1) and support from NPL. K.N. and R. M. acknowledge funding from the EPSRC Cambridge NanoDTC (Grant No. EP/G037221/1). B.B. and A.J.P. acknowledge funding from the U.K. Department of Business, Energy and Industrial Strategy (NPL Project Number 121452). J.A.-W. acknowledges the support of his Research Fellowship from Royal Commission for the Exhibition of 1851, and Royal Society Dorothy Hodgkin Research Fellowship. Y.F. also thanks Prof. Wencai Ren for the helpful discussions on the effect of pre-annealing of gold to CVD WS2. This work was carried out with the support of the Diamond Light Source, instrument B07-C (proposal SI-22123)
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