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Title: Telluride-Based Atomically Thin Layers of Ternary Two-Dimensional Transition Metal Dichalcogenide Alloys

Abstract

Alloying in two-dimensional (2D) transition metal dichalcogenides (TMDCs) has allowed band gap engineering and phase transformation, as well as modulation of electronic properties. However, most of the efforts have been focused on alloying between transition metal cations. Among those that emphasize alloying between chalcogenide anions, the sulfide–selenide combinations are popular with a few reports on selenide–telluride combinations. In this work, we show a facile chemical vapor deposition method to obtain stable alloying between selenide and telluride anions in monolayer MoSe2(1–x)Te2x alloy. These alloys retain the monolayer 2H symmetry and show good photoluminescence and band gap tunability in the near-infrared region. The nature and percentage of alloying is further confirmed and quantified via AFM, XPS, and HAADF-STEM imaging and polarized Raman spectroscopy. The stability of the two chalcogens in the monolayer 2H lattice is also consistent with thermodynamic phase mixing via DFT simulations. In conclusion, the work demonstrates a straightforward method of synthesizing telluride-based 2D TMDC alloys for further studies and emerging applications.

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [3];  [1]; ORCiD logo [3]; ORCiD logo [2];  [2]; ORCiD logo [2]; ORCiD logo [4];  [1]
  1. Rice Univ., Houston, TX (United States)
  2. Univ. of Southern California, Los Angeles, CA (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Rice Univ., Houston, TX (United States); Indian Institute of Technology, West Bengal (India)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1489547
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 20; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Apte, Amey, Krishnamoorthy, Aravind, Hachtel, Jordan Adam, Susarla, Sandhya, Idrobo, Juan Carlos, Nakano, Aiichiro, Kalia, Rajiv K., Vashishta, Priya, Tiwary, Chandra Sekhar, and Ajayan, Pulickel M. Telluride-Based Atomically Thin Layers of Ternary Two-Dimensional Transition Metal Dichalcogenide Alloys. United States: N. p., 2018. Web. doi:10.1021/acs.chemmater.8b03444.
Apte, Amey, Krishnamoorthy, Aravind, Hachtel, Jordan Adam, Susarla, Sandhya, Idrobo, Juan Carlos, Nakano, Aiichiro, Kalia, Rajiv K., Vashishta, Priya, Tiwary, Chandra Sekhar, & Ajayan, Pulickel M. Telluride-Based Atomically Thin Layers of Ternary Two-Dimensional Transition Metal Dichalcogenide Alloys. United States. https://doi.org/10.1021/acs.chemmater.8b03444
Apte, Amey, Krishnamoorthy, Aravind, Hachtel, Jordan Adam, Susarla, Sandhya, Idrobo, Juan Carlos, Nakano, Aiichiro, Kalia, Rajiv K., Vashishta, Priya, Tiwary, Chandra Sekhar, and Ajayan, Pulickel M. Wed . "Telluride-Based Atomically Thin Layers of Ternary Two-Dimensional Transition Metal Dichalcogenide Alloys". United States. https://doi.org/10.1021/acs.chemmater.8b03444. https://www.osti.gov/servlets/purl/1489547.
@article{osti_1489547,
title = {Telluride-Based Atomically Thin Layers of Ternary Two-Dimensional Transition Metal Dichalcogenide Alloys},
author = {Apte, Amey and Krishnamoorthy, Aravind and Hachtel, Jordan Adam and Susarla, Sandhya and Idrobo, Juan Carlos and Nakano, Aiichiro and Kalia, Rajiv K. and Vashishta, Priya and Tiwary, Chandra Sekhar and Ajayan, Pulickel M.},
abstractNote = {Alloying in two-dimensional (2D) transition metal dichalcogenides (TMDCs) has allowed band gap engineering and phase transformation, as well as modulation of electronic properties. However, most of the efforts have been focused on alloying between transition metal cations. Among those that emphasize alloying between chalcogenide anions, the sulfide–selenide combinations are popular with a few reports on selenide–telluride combinations. In this work, we show a facile chemical vapor deposition method to obtain stable alloying between selenide and telluride anions in monolayer MoSe2(1–x)Te2x alloy. These alloys retain the monolayer 2H symmetry and show good photoluminescence and band gap tunability in the near-infrared region. The nature and percentage of alloying is further confirmed and quantified via AFM, XPS, and HAADF-STEM imaging and polarized Raman spectroscopy. The stability of the two chalcogens in the monolayer 2H lattice is also consistent with thermodynamic phase mixing via DFT simulations. In conclusion, the work demonstrates a straightforward method of synthesizing telluride-based 2D TMDC alloys for further studies and emerging applications.},
doi = {10.1021/acs.chemmater.8b03444},
journal = {Chemistry of Materials},
number = 20,
volume = 30,
place = {United States},
year = {Wed Sep 19 00:00:00 EDT 2018},
month = {Wed Sep 19 00:00:00 EDT 2018}
}

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Figures / Tables:

Figure 1 Figure 1: Synthesis strategy of MoSe2(1‑x)Te2x monolayers: (a) Schematic of CVD growth of Te-doped MoSe2 monolayers. (b) Raman spectra of Pure MoSe2 and the Te-doped alloy samples. The increasing Te content is depicted alongside with changing morphologies of the monolayer flakes from optical micrographs (scale bars = 50 μm, 10more » μm, and 5 μm from top to bottom). (c) Photoluminescence spectra of the three samples analogous to the Raman spectra showing tunable emission characteristics from the visible to the near-infrared.« less

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.