Electron-Beam- and Thermal-Annealing-Induced Structural Transformations in Few-Layer MnPS3

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A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
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ACS Nano, Volume 17, issue 5
Quasi-two-dimensional (2D) manganese phosphorus trisulfide, MnPS3, which exhibits antiferromagnetic ordering, is a particularly interesting material in the context of magnetism in a system with reduced dimensionality and its potential technological applications. Here, we present an experimental and theoretical study on modifying the properties of freestanding MnPS3 by local structural transformations via electron irradiation in a transmission electron microscope and by thermal annealing under vacuum. In both cases we find that MnS1-xPx phases (0 ≤ x < 1) form in a crystal structure different from that of the host material, namely that of the α- or γ-MnS type. These phase transformations can both be locally controlled by the size of the electron beam as well as by the total applied electron dose and simultaneously imaged at the atomic scale. For the MnS structures generated in this process, our ab initio calculations indicate that their electronic and magnetic properties strongly depend on both in-plane crystallite orientation and thickness. Moreover, the electronic properties of the MnS phases can be further tuned by alloying with phosphorus.
Funding Information: We want to thank all cooperation associates in the framework of this manuscript. Further, we especially thank the Institut Laue-Langevin for the synthesis of the TMPT materials and Gabriele Es-Samlaoui for the preparation of TEM samples used in this work. This work was supported by the German Science Foundation (DFG), project CRC 1279 (project number 316249678), projects KR 4866/8-1, and the collaborative research center “Chemistry of Synthetic 2D Materials” SFB-1415-417590517. This work was supported by a project funded by the Carl Zeiss foundation. The computational support from the Technical University of Dresden computing cluster (TAURUS) and High-Performance Computing Center (HLRS) in Stuttgart is gratefully appreciated. M.K.K. acknowledges funding from the Deutsche Forschungsgemeinschaft (DFG) within the project DFG: KI 2546/1-1. Publisher Copyright: © 2023 The Authors. Published by American Chemical Society.
3D electron diffraction, MnPS, modification,, structural transformations, thermal annealing, α-MnS, γ-MnS
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Storm , A , Köster , J , Ghorbani-Asl , M , Kretschmer , S , Gorelik , T E , Kinyanjui , M K , Krasheninnikov , A V & Kaiser , U 2023 , ' Electron-Beam- and Thermal-Annealing-Induced Structural Transformations in Few-Layer MnPS 3 ' , ACS Nano , vol. 17 , no. 5 , pp. 4250-4260 . https://doi.org/10.1021/acsnano.2c05895