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Stabilized Synthesis of 2D Verbeekite: Monoclinic PdSe2 Crystals with High Mobility and In-Plane Optical and Electrical Anisotropy

  • Yiyi Gu
    Yiyi Gu
    Department of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States
    Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, China
    Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China
    More by Yiyi Gu
  • Lizhi Zhang
    Lizhi Zhang
    Department of Physics and Astronomy, University of Tennessee, Knoxville, Tennessee 37996, United States
    Laboratory of Theoretical and Computational Nanoscience, National Center for Nanoscience and Technology of China, Beijing 100190, China
    More by Lizhi Zhang
  • Hui Cai
    Hui Cai
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    More by Hui Cai
  • Liangbo Liang
    Liangbo Liang
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Chenze Liu
    Chenze Liu
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    More by Chenze Liu
  • Anna Hoffman
    Anna Hoffman
    Department of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States
    More by Anna Hoffman
  • Yiling Yu
    Yiling Yu
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    More by Yiling Yu
  • Austin Houston
    Austin Houston
    Department of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States
  • Alexander A. Puretzky
    Alexander A. Puretzky
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Gerd Duscher
    Gerd Duscher
    Department of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States
    More by Gerd Duscher
  • Philip D. Rack
    Philip D. Rack
    Department of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States
  • Christopher M. Rouleau
    Christopher M. Rouleau
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Xiangmin Meng
    Xiangmin Meng
    Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, China
    Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China
  • Mina Yoon
    Mina Yoon
    Materials Sciences and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    More by Mina Yoon
  • David B. Geohegan
    David B. Geohegan
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • , and 
  • Kai Xiao*
    Kai Xiao
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    *E-mail: [email protected]
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Cite this: ACS Nano 2022, 16, 9, 13900–13910
Publication Date (Web):July 1, 2022
https://doi.org/10.1021/acsnano.2c02711
Copyright © 2022 American Chemical Society

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    Abstract

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    PdSe2 has a layered structure with an unusual, puckered Cairo pentagonal tiling. Its atomic bond configuration features planar 4-fold-coordinated Pd atoms and intralayer Se–Se bonds that enable polymorphic phases with distinct electronic and quantum properties, especially when atomically thin. PdSe2 is conventionally orthorhombic, and direct synthesis of its metastable polymorphic phases is still a challenge. Here, we report an ambient-pressure chemical vapor deposition approach to synthesize metastable monoclinic PdSe2. Monoclinic PdSe2 is shown to be synthesized selectively under Se-deficient conditions that induce Se vacancies. These defects are shown by first-principles density functional theory calculations to reduce the free energy of the metastable monoclinic phase, thereby stabilizing it during synthesis. The structure and composition of the monoclinic PdSe2 crystals are identified and characterized by scanning transmission electron microscopy imaging, convergent beam electron diffraction, and electron energy loss spectroscopy. Polarized Raman spectroscopy of the monoclinic PdSe2 flakes reveals their strong in-plane optical anisotropy. Electrical transport measurements show that the monoclinic PdSe2 exhibits n-type charge carrier conduction with electron mobilities up to ∼298 cm2 V–1 s–1 and a strong in-plane electron mobility anisotropy of ∼1.9. The defect-mediated growth pathway identified in this work is promising for phase-selective direct synthesis of other 2D transition metal dichalcogenides.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsnano.2c02711.

    • Theoretical calculation of the Raman scattering mode of PdSe2, atomic structures and optical images of both O- and M-PdSe2 flakes grown on different substrates, low-magnification TEM image of M-PdSe2 flakes on a TEM grid, Raman spectra of O-PdSe2 and M-PdSe2 grown on SiO2 substrates, first-principles calculations for the electronic band structure of monolayer and bulk M-PdSe2, calculated in-plane elastic moduli (C2D), effective masses (m*), deformation potentials (Ed), and carrier mobilities (μ) along the x and y directions for the bulk M-PdSe2, Raman and AFM characterizations of the M-PdSe2 flake in a fabricated FET device, output curves of an M-PdSe2 device at different temperatures, and electrical transport of an M-PdSe2 device (PDF)

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    Cited By

    This article is cited by 8 publications.

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    2. Tadasha Jena, Garima Choudhary, Md Tarik Hossain, Upasana Nath, Manabendra Sarma, P. K. Giri. Salt-Catalyzed Directed Growth of Bilayer Palladium Diselenide (PdSe2) Dendrites and Pd Nanoparticle-Decorated PdSe2–Pd2Se3 Junction Exhibiting Very High Surface Enhanced Raman Scattering Sensitivity. Chemistry of Materials 2024, Article ASAP.
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