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Title: Tuning Electronic Structure of Single Layer MoS 2 through Defect and Interface Engineering

Abstract

Transition-metal dichalcogenides (TMDs) have emerged in recent years as a special group of two-dimensional materials and have attracted tremendous attention. Among these TMD materials, molybdenum disulfide (MoS2) has shown promising applications in electronics, photonics, energy, and electrochemistry. In particular, the defects in MoS2 play an essential role in altering the electronic, magnetic, optical, and catalytic properties of MoS2, presenting a useful way to engineer the performance of MoS2. The mechanisms by which lattice defects affect the MoS2 properties are unsettled. In this work, we reveal systematically how lattice defects and substrate interface affect MoS2 electronic structure. We fabricated single-layer MoS2 by chemical vapor deposition and then transferred onto Au, single-layer graphene, hexagonal boron nitride, and CeO2 as substrates and created defects in MoS2 by ion irradiation. Here, we assessed how these defects and substrates affect the electronic structure of MoS2 by performing X-ray photoelectron spectroscopy, Raman and photoluminescence spectroscopies, and scanning tunneling microscopy/spectroscopy measurements. Molecular dynamics and first-principles based simulations allowed us to conclude the predominant lattice defects upon ion irradiation and associate those with the experimentally obtained electronic structure. We found that the substrates can tune the electronic energy levels in MoS2 due to charge transfer at the interface.more » Furthermore, the reduction state of CeO2 as an oxide substrate affects the interface charge transfer with MoS2. The irradiated MoS2 had a faster hydrogen evolution kinetics compared to the as-prepared MoS2, demonstrating the concept of defect controlled reactivity in this phase. Our findings provide effective probes for energy band and defects in MoS2 and show the importance of defect engineering in tuning the functionalities of MoS2 and other TMDs in electronics, optoelectronics, and electrochemistry.« less

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [3];  [4];  [5]; ORCiD logo [6];  [4];  [7]; ORCiD logo [8];  [9]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Nuclear Science and Engineering, Research Lab. of Electronics; South China Univ. of Technology, Guangzhou, Guangdong (China)
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Electrical Engineering and Computer Science; Pennsylvania State Univ., University Park, PA (United States). Dept. of Electrical Engineering
  3. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Research Lab. of Electronics
  4. Peking Univ., Beijing (China). School of Physics, State Key Lab. of Nuclear Physics and Technology, School of Physics
  5. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Electrical Engineering and Computer Science; Boston Univ., MA (United States). Dept. of Chemistry, Division of Materials Science and Engineering, and The Photonics Center
  6. Peking Univ., Shenzhen (China). School of Advanced Materials, Shenzhen Graduate School
  7. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Electrical Engineering and Computer Science, and Dept. of Physics
  8. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Research Lab. of Electronics; Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Electrical Engineering and Computer Science
  9. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Nuclear Science and Engineering, and Dept. of Material Science and Engineering
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE). Solid-State Solar-Thermal Energy Conversion Center (S3TEC); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1539576
Grant/Contract Number:  
SC0001088; SC0001299; SC0002633
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 12; Journal Issue: 3; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING; Chemistry; Science & Technology - Other Topics; Materials Science; transition-metal dichalcogenides; hydrogen evolution reaction; ion irradiation; X-ray photoelectron spectroscopy; Raman spectroscopy; scanning tunneling microscopy

Citation Formats

Chen, Yan, Huang, Shengxi, Ji, Xiang, Adepalli, Kiran, Yin, Kedi, Ling, Xi, Wang, Xinwei, Xue, Jianmin, Dresselhaus, Mildred, Kong, Jing, and Yildiz, Bilge. Tuning Electronic Structure of Single Layer MoS 2 through Defect and Interface Engineering. United States: N. p., 2018. Web. doi:10.1021/acsnano.7b08418.
Chen, Yan, Huang, Shengxi, Ji, Xiang, Adepalli, Kiran, Yin, Kedi, Ling, Xi, Wang, Xinwei, Xue, Jianmin, Dresselhaus, Mildred, Kong, Jing, & Yildiz, Bilge. Tuning Electronic Structure of Single Layer MoS 2 through Defect and Interface Engineering. United States. doi:10.1021/acsnano.7b08418.
Chen, Yan, Huang, Shengxi, Ji, Xiang, Adepalli, Kiran, Yin, Kedi, Ling, Xi, Wang, Xinwei, Xue, Jianmin, Dresselhaus, Mildred, Kong, Jing, and Yildiz, Bilge. Sat . "Tuning Electronic Structure of Single Layer MoS 2 through Defect and Interface Engineering". United States. doi:10.1021/acsnano.7b08418. https://www.osti.gov/servlets/purl/1539576.
@article{osti_1539576,
title = {Tuning Electronic Structure of Single Layer MoS 2 through Defect and Interface Engineering},
author = {Chen, Yan and Huang, Shengxi and Ji, Xiang and Adepalli, Kiran and Yin, Kedi and Ling, Xi and Wang, Xinwei and Xue, Jianmin and Dresselhaus, Mildred and Kong, Jing and Yildiz, Bilge},
abstractNote = {Transition-metal dichalcogenides (TMDs) have emerged in recent years as a special group of two-dimensional materials and have attracted tremendous attention. Among these TMD materials, molybdenum disulfide (MoS2) has shown promising applications in electronics, photonics, energy, and electrochemistry. In particular, the defects in MoS2 play an essential role in altering the electronic, magnetic, optical, and catalytic properties of MoS2, presenting a useful way to engineer the performance of MoS2. The mechanisms by which lattice defects affect the MoS2 properties are unsettled. In this work, we reveal systematically how lattice defects and substrate interface affect MoS2 electronic structure. We fabricated single-layer MoS2 by chemical vapor deposition and then transferred onto Au, single-layer graphene, hexagonal boron nitride, and CeO2 as substrates and created defects in MoS2 by ion irradiation. Here, we assessed how these defects and substrates affect the electronic structure of MoS2 by performing X-ray photoelectron spectroscopy, Raman and photoluminescence spectroscopies, and scanning tunneling microscopy/spectroscopy measurements. Molecular dynamics and first-principles based simulations allowed us to conclude the predominant lattice defects upon ion irradiation and associate those with the experimentally obtained electronic structure. We found that the substrates can tune the electronic energy levels in MoS2 due to charge transfer at the interface. Furthermore, the reduction state of CeO2 as an oxide substrate affects the interface charge transfer with MoS2. The irradiated MoS2 had a faster hydrogen evolution kinetics compared to the as-prepared MoS2, demonstrating the concept of defect controlled reactivity in this phase. Our findings provide effective probes for energy band and defects in MoS2 and show the importance of defect engineering in tuning the functionalities of MoS2 and other TMDs in electronics, optoelectronics, and electrochemistry.},
doi = {10.1021/acsnano.7b08418},
journal = {ACS Nano},
number = 3,
volume = 12,
place = {United States},
year = {2018},
month = {2}
}

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Works referencing / citing this record:

Defect engineering of molybdenum disulfide through ion irradiation to boost hydrogen evolution reaction performance
journal, April 2019


Basal plane oxygen exchange of epitaxial MoS 2 without edge oxidation
journal, July 2019

  • Grønborg, Signe S.; Thorarinsdottir, Kristbjörg; Kyhl, Line
  • 2D Materials, Vol. 6, Issue 4
  • DOI: 10.1088/2053-1583/ab2d00

Defect engineering of molybdenum disulfide through ion irradiation to boost hydrogen evolution reaction performance
journal, April 2019


Basal plane oxygen exchange of epitaxial MoS 2 without edge oxidation
journal, July 2019

  • Grønborg, Signe S.; Thorarinsdottir, Kristbjörg; Kyhl, Line
  • 2D Materials, Vol. 6, Issue 4
  • DOI: 10.1088/2053-1583/ab2d00