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Title: Multimodal spectromicroscopy of monolayer WS 2 enabled by ultra-clean van der Waals epitaxy

Abstract

Van der Waals epitaxy enables the integration of 2D transition metal dichalcogenides with other layered materials to form heterostructures with atomically sharp interfaces. However, the ability to fully utilize and understand these materials using surface science techniques such as angle resolved photoemission spectroscopy (ARPES) and scanning tunneling microscopy (STM) requires low defect, large area, epitaxial coverage with ultra-clean interfaces. We have developed a chemical vapor deposition van der Waals epitaxy growth process where the metal and chalcogen sources are separated such that growth times can be extended significantly to yield high coverage while minimizing surface contamination. We also demonstrate the growth of high quality 2D WS 2 over large areas on graphene. The as-grown vertical heterostructures are exceptionally clean as demonstrated by ARPES, STM and spatially resolved photoluminescence mapping. With these correlated techniques we are able to relate defect density to electronic band structure and, ultimately, optical properties. We find that our synthetic approach provides ultra-clean, low defect density (~10 12 cm -2), ~10 μm large WS 2 monolayer crystals, with an electronic band structure and valence band effective masses that perfectly match the theoretical prediction for pristine WS 2.

Authors:
; ; ORCiD logo; ; ; ; ; ; ; ; ; ORCiD logo
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division; Swiss National Science Foundation (SNSF)
OSTI Identifier:
1461592
Alternate Identifier(s):
OSTI ID: 1465470
Grant/Contract Number:  
[AC02-05CH11231; P2SKP2_171770]
Resource Type:
Published Article
Journal Name:
2D Materials
Additional Journal Information:
[Journal Name: 2D Materials Journal Volume: 5 Journal Issue: 4]; Journal ID: ISSN 2053-1583
Publisher:
IOP Publishing
Country of Publication:
United Kingdom
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; transition metal dichalcogenides; TMD; TMDC; chemical vapor deposition; effective mass; exciton

Citation Formats

Kastl, C., Chen, C. T., Koch, R. J., Schuler, B., Kuykendall, T. R., Bostwick, A., Jozwiak, C., Seyller, T., Rotenberg, E., Weber-Bargioni, A., Aloni, S., and Schwartzberg, A. M. Multimodal spectromicroscopy of monolayer WS 2 enabled by ultra-clean van der Waals epitaxy. United Kingdom: N. p., 2018. Web. doi:10.1088/2053-1583/aad21c.
Kastl, C., Chen, C. T., Koch, R. J., Schuler, B., Kuykendall, T. R., Bostwick, A., Jozwiak, C., Seyller, T., Rotenberg, E., Weber-Bargioni, A., Aloni, S., & Schwartzberg, A. M. Multimodal spectromicroscopy of monolayer WS 2 enabled by ultra-clean van der Waals epitaxy. United Kingdom. doi:10.1088/2053-1583/aad21c.
Kastl, C., Chen, C. T., Koch, R. J., Schuler, B., Kuykendall, T. R., Bostwick, A., Jozwiak, C., Seyller, T., Rotenberg, E., Weber-Bargioni, A., Aloni, S., and Schwartzberg, A. M. Wed . "Multimodal spectromicroscopy of monolayer WS 2 enabled by ultra-clean van der Waals epitaxy". United Kingdom. doi:10.1088/2053-1583/aad21c.
@article{osti_1461592,
title = {Multimodal spectromicroscopy of monolayer WS 2 enabled by ultra-clean van der Waals epitaxy},
author = {Kastl, C. and Chen, C. T. and Koch, R. J. and Schuler, B. and Kuykendall, T. R. and Bostwick, A. and Jozwiak, C. and Seyller, T. and Rotenberg, E. and Weber-Bargioni, A. and Aloni, S. and Schwartzberg, A. M.},
abstractNote = {Van der Waals epitaxy enables the integration of 2D transition metal dichalcogenides with other layered materials to form heterostructures with atomically sharp interfaces. However, the ability to fully utilize and understand these materials using surface science techniques such as angle resolved photoemission spectroscopy (ARPES) and scanning tunneling microscopy (STM) requires low defect, large area, epitaxial coverage with ultra-clean interfaces. We have developed a chemical vapor deposition van der Waals epitaxy growth process where the metal and chalcogen sources are separated such that growth times can be extended significantly to yield high coverage while minimizing surface contamination. We also demonstrate the growth of high quality 2D WS2 over large areas on graphene. The as-grown vertical heterostructures are exceptionally clean as demonstrated by ARPES, STM and spatially resolved photoluminescence mapping. With these correlated techniques we are able to relate defect density to electronic band structure and, ultimately, optical properties. We find that our synthetic approach provides ultra-clean, low defect density (~1012 cm-2), ~10 μm large WS2 monolayer crystals, with an electronic band structure and valence band effective masses that perfectly match the theoretical prediction for pristine WS2.},
doi = {10.1088/2053-1583/aad21c},
journal = {2D Materials},
number = [4],
volume = [5],
place = {United Kingdom},
year = {2018},
month = {7}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1088/2053-1583/aad21c

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Cited by: 6 works
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Works referenced in this record:

Controlling sulphur precursor addition for large single crystal domains of WS 2
journal, January 2014


Visualizing nanoscale excitonic relaxation properties of disordered edges and grain boundaries in monolayer molybdenum disulfide
journal, August 2015

  • Bao, Wei; Borys, Nicholas J.; Ko, Changhyun
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8993

Scalable synthesis of WS 2 on graphene and h-BN: an all-2D platform for light-matter transduction
journal, September 2016


Recent Advances in Controlling Syntheses and Energy Related Applications of MX 2 and MX 2 /Graphene Heterostructures
journal, April 2016

  • Shi, Jianping; Ji, Qingqing; Liu, Zhongfan
  • Advanced Energy Materials, Vol. 6, Issue 17
  • DOI: 10.1002/aenm.201600459

Oxygen-Assisted Chemical Vapor Deposition Growth of Large Single-Crystal and High-Quality Monolayer MoS 2
journal, December 2015

  • Chen, Wei; Zhao, Jing; Zhang, Jing
  • Journal of the American Chemical Society, Vol. 137, Issue 50
  • DOI: 10.1021/jacs.5b10519

Graphene Nucleation on Transition Metal Surface: Structure Transformation and Role of the Metal Step Edge
journal, April 2011

  • Gao, Junfeng; Yip, Joanne; Zhao, Jijun
  • Journal of the American Chemical Society, Vol. 133, Issue 13, p. 5009-5015
  • DOI: 10.1021/ja110927p

Optical Absorption of a Few Unit-Cell Layers of Mo S 2
journal, October 1965


Unraveling the Structural and Electronic Properties at the WSe 2 –Graphene Interface for a Rational Design of van der Waals Heterostructures
journal, February 2018

  • Agnoli, Stefano; Ambrosetti, Alberto; Menteş, Tevfik Onur
  • ACS Applied Nano Materials, Vol. 1, Issue 3
  • DOI: 10.1021/acsanm.7b00315

Spatially Resolved Electronic Properties of Single-Layer WS 2 on Transition Metal Oxides
journal, October 2016


Charge density wave order in 1D mirror twin boundaries of single-layer MoSe2
journal, April 2016

  • Barja, Sara; Wickenburg, Sebastian; Liu, Zhen-Fei
  • Nature Physics, Vol. 12, Issue 8
  • DOI: 10.1038/nphys3730

STM study of the MoS2 flakes grown on graphite: A model system for atomically clean 2D heterostructure interfaces
journal, August 2016


Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides
journal, March 2016


Optically Discriminating Carrier-Induced Quasiparticle Band Gap and Exciton Energy Renormalization in Monolayer MoS 2
journal, August 2017


Fluorescence Concentric Triangles: A Case of Chemical Heterogeneity in WS 2 Atomic Monolayer
journal, August 2016


Strain and structure heterogeneity in MoS2 atomic layers grown by chemical vapour deposition
journal, November 2014

  • Liu, Zheng; Amani, Matin; Najmaei, Sina
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms6246

Anomalous Above-Gap Photoexcitations and Optical Signatures of Localized Charge Puddles in Monolayer Molybdenum Disulfide
journal, February 2017


Atomically Thin Heterostructures Based on Single-Layer Tungsten Diselenide and Graphene
journal, November 2014

  • Lin, Yu-Chuan; Chang, Chih-Yuan S.; Ghosh, Ram Krishna
  • Nano Letters, Vol. 14, Issue 12
  • DOI: 10.1021/nl503144a

Layer-Controlled, Wafer-Scale, and Conformal Synthesis of Tungsten Disulfide Nanosheets Using Atomic Layer Deposition
journal, November 2013

  • Song, Jeong-Gyu; Park, Jusang; Lee, Wonseon
  • ACS Nano, Vol. 7, Issue 12
  • DOI: 10.1021/nn405194e

Growth and Optical Properties of High-Quality Monolayer WS 2 on Graphite
journal, February 2015


Direct exciton emission from atomically thin transition metal dichalcogenide heterostructures near the lifetime limit
journal, September 2017


Shape Evolution of Monolayer MoS 2 Crystals Grown by Chemical Vapor Deposition
journal, November 2014

  • Wang, Shanshan; Rong, Youmin; Fan, Ye
  • Chemistry of Materials, Vol. 26, Issue 22
  • DOI: 10.1021/cm5025662

Large-area MoS 2 grown using H 2 S as the sulphur source
journal, November 2015


Controlled Preferential Oxidation of Grain Boundaries in Monolayer Tungsten Disulfide for Direct Optical Imaging
journal, February 2015


Ultrasharp interfaces grown with Van der Waals epitaxy
journal, August 1986


All Chemical Vapor Deposition Growth of MoS 2 :h-BN Vertical van der Waals Heterostructures
journal, April 2015


Edge conduction in monolayer WTe2
journal, April 2017

  • Fei, Zaiyao; Palomaki, Tauno; Wu, Sanfeng
  • Nature Physics, Vol. 13, Issue 7
  • DOI: 10.1038/nphys4091

Electronic properties of single-layer tungsten disulfide on epitaxial graphene on silicon carbide
journal, January 2017

  • Forti, Stiven; Rossi, Antonio; Büch, Holger
  • Nanoscale, Vol. 9, Issue 42
  • DOI: 10.1039/C7NR05495E

Giant spin-splitting and gap renormalization driven by trions in single-layer WS2/h-BN heterostructures
journal, January 2018


Electronics based on two-dimensional materials
journal, October 2014

  • Fiori, Gianluca; Bonaccorso, Francesco; Iannaccone, Giuseppe
  • Nature Nanotechnology, Vol. 9, Issue 10
  • DOI: 10.1038/nnano.2014.207

Optoelectronic Devices Based on Atomically Thin Transition Metal Dichalcogenides
journal, March 2016

  • Pospischil, Andreas; Mueller, Thomas
  • Applied Sciences, Vol. 6, Issue 3
  • DOI: 10.3390/app6030078

Direct Chemical Vapor Deposition Growth of WS 2 Atomic Layers on Hexagonal Boron Nitride
journal, July 2014

  • Okada, Mitsuhiro; Sawazaki, Takumi; Watanabe, Kenji
  • ACS Nano, Vol. 8, Issue 8
  • DOI: 10.1021/nn503093k

Realizing Large-Scale, Electronic-Grade Two-Dimensional Semiconductors
journal, January 2018


Titanium Disulfide Coated Carbon Nanotube Hybrid Electrodes Enable High Energy Density Symmetric Pseudocapacitors
journal, December 2017


A library of atomically thin metal chalcogenides
journal, April 2018


van der Waals epitaxy: 2D materials and topological insulators
journal, December 2017


Hydrogen evolution activity of individual mono-, bi-, and few-layer MoS 2 towards photocatalysis
journal, September 2017


Point Defects and Grain Boundaries in Rotationally Commensurate MoS 2 on Epitaxial Graphene
journal, March 2016

  • Liu, Xiaolong; Balla, Itamar; Bergeron, Hadallia
  • The Journal of Physical Chemistry C, Vol. 120, Issue 37
  • DOI: 10.1021/acs.jpcc.6b02073

Coulomb engineering of the bandgap and excitons in two-dimensional materials
journal, May 2017

  • Raja, Archana; Chaves, Andrey; Yu, Jaeeun
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms15251

Growth and electronic structure of epitaxial single-layer WS 2 on Au(111)
journal, December 2015


Rotationally Commensurate Growth of MoS 2 on Epitaxial Graphene
journal, November 2015


The important role of water in growth of monolayer transition metal dichalcogenides
journal, March 2017


Molecular Beam Epitaxy of Highly Crystalline Monolayer Molybdenum Disulfide on Hexagonal Boron Nitride
journal, July 2017

  • Fu, Deyi; Zhao, Xiaoxu; Zhang, Yu-Yang
  • Journal of the American Chemical Society, Vol. 139, Issue 27
  • DOI: 10.1021/jacs.7b05131

Towards wafer-size graphene layers by atmospheric pressure graphitization of silicon carbide
journal, February 2009

  • Emtsev, Konstantin V.; Bostwick, Aaron; Horn, Karsten
  • Nature Materials, Vol. 8, Issue 3
  • DOI: 10.1038/nmat2382

Wafer-Scale Growth and Transfer of Highly-Oriented Monolayer MoS 2 Continuous Films
journal, October 2016


Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor
journal, August 2014

  • Ugeda, Miguel M.; Bradley, Aaron J.; Shi, Su-Fei
  • Nature Materials, Vol. 13, Issue 12
  • DOI: 10.1038/nmat4061

Nature of Electronic States in Atomically Thin MoS2 Field-Effect Transistors
journal, October 2011

  • Ghatak, Subhamoy; Pal, Atindra Nath; Ghosh, Arindam
  • ACS Nano, Vol. 5, Issue 10, p. 7707-7712
  • DOI: 10.1021/nn202852j

van der Waals Epitaxy of MoS2 Layers Using Graphene As Growth Templates
journal, May 2012

  • Shi, Yumeng; Zhou, Wu; Lu, Ang-Yu
  • Nano Letters, Vol. 12, Issue 6, p. 2784-2791
  • DOI: 10.1021/nl204562j

    Works referencing / citing this record:

    Doping of Two-Dimensional Semiconductors: A Rapid Review and Outlook
    journal, January 2019