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      Sonication-assisted liquid phase exfoliation of two-dimensional CrTe 3 under inert conditions

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          Abstract

          Liquid phase exfoliation (LPE) has been used for the successful fabrication of nanosheets from a large number of van der Waals materials. While this allows to study fundamental changes of material properties’ associated with reduced dimensions, it also changes the chemistry of many materials due to a significant increase of the effective surface area, often accompanied with enhanced reactivity and accelerated oxidation. To prevent material decomposition, LPE and processing in inert atmosphere have been developed, which enables the preparation of pristine nanomaterials, and to systematically study compositional changes over time for different storage conditions. Here, we demonstrate the inert exfoliation of the oxidation-sensitive van der Waals crystal, CrTe 3. The pristine nanomaterial was purified and size-selected by centrifugation, nanosheet dimensions in the fractions quantified by atomic force microscopy and studied by Raman, X-ray photoelectron spectroscopy (XPS), energy-dispersive X-ray spectroscopy (EDX) and photo spectroscopic measurements. We find a dependence of the relative intensities of the CrTe 3 Raman modes on the propagation direction of the incident light, which prevents a correlation of the Raman spectral profile to the nanosheet dimensions. XPS and EDX reveal that the contribution of surface oxides to the spectra is reduced after exfoliation compared to the bulk material. Further, the decomposition mechanism of the nanosheets was studied by time-dependent extinction measurements after water titration experiments to initially dry solvents, which suggest that water plays a significant role in the material decomposition.

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          Computational search for magnetic and non-magnetic 2D topological materials using unified spin–orbit spillage screening

          Two-dimensional topological materials (2D TMs) have a variety of properties that make them attractive for applications including spintronics and quantum computation. However, there are only a few such experimentally known materials. To help discover new 2D TMs, we develop a unified and computationally inexpensive approach to identify magnetic and non-magnetic 2D TMs, including gapped and semi-metallic topological classifications, in a high-throughput way using density functional theory-based spin–orbit spillage, Wannier-interpolation, and related techniques. We first compute the spin–orbit spillage for the ~1000 2D materials in the JARVIS-DFT dataset, resulting in 122 materials with high-spillage values. Then, we use Wannier-interpolation to carry-out Z 2 , Chern-number, anomalous Hall conductivity, Curie temperature, and edge state calculations to further support the predictions. We identify various topologically non-trivial classes such as quantum spin-Hall insulators, quantum anomalous-Hall insulators, and semimetals. For a few predicted materials, we run G 0 W 0 +SOC and DFT+U calculations. We find that as we introduce many-body effects, only a few materials retain non-trivial band-topology, suggesting the importance of high-level density functional theory (DFT) methods in predicting 2D topological materials. However, as an initial step, the automated spillage screening and Wannier-approach provide useful predictions for finding new topological materials and to narrow down candidates for experimental synthesis and characterization.
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            Author and article information

            Contributors
            Journal
            Ultrason Sonochem
            Ultrason Sonochem
            Ultrasonics Sonochemistry
            Elsevier
            1350-4177
            1873-2828
            19 July 2023
            August 2023
            19 July 2023
            : 98
            : 106528
            Affiliations
            [a ]Institute of Physical Chemistry, Heidelberg University, Im Neuenheimer Feld 253, 69120 Heidelberg, Germany
            [b ]School of Physics, University of Dublin, Trinity College, Dublin 2, Ireland
            [c ]Institute for Solid-State Physics, Technische Universität Berlin, Hardenbergstraße 36, 10623 Berlin, Germany
            [d ]Department of Physics, Friedrich-Alexander-Universität Erlangen-Nürnberg, Staudtstr. 7, 91058 Erlangen, Germany
            [e ]Chair for Emerging Electronic Technologies, TU Dresden, Nöthnitzer Str. 61, Dresden, 01187 Sachsen, Germany
            [f ]Leibniz-Institute for Solid State and Materials Research Dresden, Helmholtzstraße 20, Dresden 01069, Sachsen, Germany
            [g ]Institute for Applied Materials—Energy Storage Systems (IAM-ESS), Karlsruhe Institute of Technology (KIT), 76344 Eggenstein, Germany
            [h ]Paul-Drude-Institut für Festkörperelektronik, Leibniz-Institut im Forschungsverbund Berlin e.V, Hausvogteiplatz 5–7, 10117 Berlin, Germany
            [i ]Institute of Inorganic Chemistry, University of Kiel, Max-Eyth-Straße 2, 24118 Kiel, Germany
            [j ]Chair of Physical Chemistry of Nanomaterials, University of Kassel, Heinrich-Plett-Straße 40, 34132 Kassel, Germany
            Author notes
            [* ]Corresponding author. backes@ 123456uni-kassel.de
            Article
            S1350-4177(23)00240-7 106528
            10.1016/j.ultsonch.2023.106528
            10407284
            39179213-7951-45d3-b6bc-b8e279d546a9
            © 2023 The Author(s)

            This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

            History
            : 18 April 2023
            : 9 July 2023
            : 17 July 2023
            Categories
            Original Research Article

            liquid phase exfoliation,sonication,2d materials,degradation

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