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    Substrate influence on transition metal dichalcogenide monolayer exciton absorption linewidth broadening

    Fuhui Shao1,2,3, Steffi Y. Woo1, Nianjheng Wu1,4, Robert Schneider5, Andrew J. Mayne4, Steffen Michaelis de Vasconcellos5, Ashish Arora5,6, Benjamin J. Carey5, Johann A. Preuß5 et al.

    Noémie Bonnet1, Mauro Och7, Cecilia Mattevi7, Kenji Watanabe8, Takashi Taniguchi9, Zhichuan Niu2,3, Rudolf Bratschitsch5, and Luiz H. G. Tizei1,*

    • 1Université Paris-Saclay, CNRS, Laboratoire de Physique des Solides, 91405 Orsay, France
    • 2State Key Laboratory for Superlattices and Microstructures, Institute of Semiconductors, Chinese Academy of Sciences, Beijing 100083, China
    • 3College of Materials Science and Opto-Electronic Technology, University of Chinese Academy of Sciences, Beijing 100083, China
    • 4Université Paris-Saclay, CNRS, Institut des Sciences Moléculaires d'Orsay, 91405 Orsay, France
    • 5Institute of Physics and Center for Nanotechnology, University of Münster, Wilhelm-Klemm-Straße 10, 48149 Münster, Germany
    • 6Indian Institute of Science Education and Research, Dr. Homi Bhabha Road, 411008 Pune, India
    • 7Department of Materials, Imperial College London, London SW7 2AZ, United Kingdom
    • 8Research Center for Functional Materials, National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan
    • 9International Center for Materials Nanoarchitectonics, National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan

    • *luiz.galvao-tizei@universite-paris-saclay.fr

    Phys. Rev. Materials 6, 074005 – Published 22 July, 2022

    DOI: https://doi.org/10.1103/PhysRevMaterials.6.074005

    Abstract

    The excitonic states of transition metal dichalcogenide (TMD) monolayers are heavily influenced by their external dielectric environment and depend on the substrate used. In this work, various wide band gap dielectric materials, namely hexagonal boron nitride (h−BN) and amorphous silicon nitride (Si3N4), under different configurations as support or encapsulation material for WS2 monolayers, are investigated to disentangle the factors contributing to inhomogeneous broadening of exciton absorption lines in TMDs using electron energy loss spectroscopy in a scanning transmission electron microscope. In addition, monolayer roughness in each configuration was determined from tilt series of electron diffraction patterns by assessing the broadening of diffraction spots by comparison with simulations. From our experiments, the main factors that play a role in linewidth broadening can be classified, in increasing order of importance, by monolayer roughness, surface cleanliness, and substrate-induced charge trapping. Furthermore, because high-energy electrons are used as a probe, electron-beam-induced damage on bare TMD monolayers is also revealed to be responsible for irreversible linewidth increases. h−BN not only provides clean surfaces of TMD monolayers and minimal charge disorder, but can also protect the TMD from irradiation damage. This work provides a better understanding of the mechanisms by which h−BN remains, to date, the most compatible material for 2D material encapsulation, facilitating the realization of intrinsic material properties to their full potential.

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