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Title: Thermally Induced 2D Alloy-Heterostructure Transformation in Quaternary Alloys

Abstract

Composition and phase specific 2D transition metal dichalogenides (2D TMDs) with a controlled electronic and chemical structure are essential for future electronics. While alloying allows bandgap tunability, heterostructure formation creates atomically sharp electronic junctions. Herein, the formation of lateral heterostructures from quaternary 2D TMD alloys, by thermal annealing, is demonstrated. Phase separation is observed through photoluminescence and Raman spectroscopy, and the sharp interface of the lateral heterostructure is examined via scanning transmission electron microscopy. The composition–dependent transformation is caused by existence of miscibility gap in the quaternary alloys. The phase diagram displaying the miscibility gap is obtained from the reciprocal solution model based on density functional theory and verified experimentally. In conclusion, the experiments show direct evidence of composition–driven heterostructure formation in 2D atomic layer systems.

Authors:
 [1]; ORCiD logo [2];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [2];  [1];  [1]; ORCiD logo [3];  [1]
  1. Rice Univ., Houston, TX (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. 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:
1493999
Alternate Identifier(s):
OSTI ID: 1469232
Grant/Contract Number:  
AC05-00OR22725; SC0012547
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 45; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; alloys; density functional theory; heterostructures; phase diagrams; phase stability; scanning transmission electron microscopy

Citation Formats

Susarla, Sandhya, Hachtel, Jordan A., Yang, Xiting, Kutana, Alex, Apte, Amey, Jin, Zehua, Vajtai, Robert, Idrobo, Juan Carlos, Lou, Jun, Yakobson, Boris I., Tiwary, Chandra Sekhar, and Ajayan, Pulickel M. Thermally Induced 2D Alloy-Heterostructure Transformation in Quaternary Alloys. United States: N. p., 2018. Web. doi:10.1002/adma.201804218.
Susarla, Sandhya, Hachtel, Jordan A., Yang, Xiting, Kutana, Alex, Apte, Amey, Jin, Zehua, Vajtai, Robert, Idrobo, Juan Carlos, Lou, Jun, Yakobson, Boris I., Tiwary, Chandra Sekhar, & Ajayan, Pulickel M. Thermally Induced 2D Alloy-Heterostructure Transformation in Quaternary Alloys. United States. doi:10.1002/adma.201804218.
Susarla, Sandhya, Hachtel, Jordan A., Yang, Xiting, Kutana, Alex, Apte, Amey, Jin, Zehua, Vajtai, Robert, Idrobo, Juan Carlos, Lou, Jun, Yakobson, Boris I., Tiwary, Chandra Sekhar, and Ajayan, Pulickel M. Mon . "Thermally Induced 2D Alloy-Heterostructure Transformation in Quaternary Alloys". United States. doi:10.1002/adma.201804218. https://www.osti.gov/servlets/purl/1493999.
@article{osti_1493999,
title = {Thermally Induced 2D Alloy-Heterostructure Transformation in Quaternary Alloys},
author = {Susarla, Sandhya and Hachtel, Jordan A. and Yang, Xiting and Kutana, Alex and Apte, Amey and Jin, Zehua and Vajtai, Robert and Idrobo, Juan Carlos and Lou, Jun and Yakobson, Boris I. and Tiwary, Chandra Sekhar and Ajayan, Pulickel M.},
abstractNote = {Composition and phase specific 2D transition metal dichalogenides (2D TMDs) with a controlled electronic and chemical structure are essential for future electronics. While alloying allows bandgap tunability, heterostructure formation creates atomically sharp electronic junctions. Herein, the formation of lateral heterostructures from quaternary 2D TMD alloys, by thermal annealing, is demonstrated. Phase separation is observed through photoluminescence and Raman spectroscopy, and the sharp interface of the lateral heterostructure is examined via scanning transmission electron microscopy. The composition–dependent transformation is caused by existence of miscibility gap in the quaternary alloys. The phase diagram displaying the miscibility gap is obtained from the reciprocal solution model based on density functional theory and verified experimentally. In conclusion, the experiments show direct evidence of composition–driven heterostructure formation in 2D atomic layer systems.},
doi = {10.1002/adma.201804218},
journal = {Advanced Materials},
issn = {0935-9648},
number = 45,
volume = 30,
place = {United States},
year = {2018},
month = {9}
}

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