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Title: Evolution of Metastable Defects and Its Effect on the Electronic Properties of MoS2 Films

Journal Article · · Scientific Reports
 [1];  [2]; ORCiD logo [3];  [4];  [5];  [6];  [7];  [8];  [4];  [4]; ORCiD logo [2]
  1. Drexel Univ., Philadelphia, PA (United States); Slovak Academy of Sciences, Bratislava (Slovak Republic)
  2. Drexel Univ., Philadelphia, PA (United States)
  3. Temple Univ., Philadelphia, PA (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Temple Univ., Philadelphia, PA (United States)
  5. Temple Univ., Philadelphia, PA (United States); Institute for Physics of Microstructure RAS, Novgorod (Russia)
  6. Temple Univ., Philadelphia, PA (United States); Univ. of Salerno, Fisciano (SA) (Italy)
  7. Temple Univ., Philadelphia, PA (United States); Univ. of San Francisco, San Francisco, CA (United States)
  8. Brookhaven National Lab. (BNL), Upton, NY (United States)

Here, we report on structural and electronic properties of defects in chemical vapor-deposited monolayer and few-layer MoS2 films. Scanning tunneling microscopy, Kelvin probe force microscopy, and transmission electron microscopy were used to obtain high resolution images and quantitative measurements of the local density of states, work function and nature of defects in MoS2 films. We track the evolution of defects that are formed under heating and electron beam irradiation. We observe formation of metastable domains with different work function values after annealing the material in ultra-high vacuum to moderate temperatures. We attribute these metastable values of the work function to evolution of crystal defects forming during the annealing. The experiments show that sulfur vacancies formed after exposure to elevated temperatures diffuse, coalesce, and migrate bringing the system from a metastable to equilibrium ground state. The process could be thermally or e-beam activated with estimated energy barrier for sulfur vacancy migration of 0.6 eV in single unit cell MoS2. Even at equilibrium conditions, the work function and local density of states values are strongly affected near grain boundaries and edges. The results provide initial estimates of the thermal budgets available for reliable fabrication of MoS2-based integrated electronics and indicate the importance of defect control and layer passivation.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Complex Materials from First Principles (CCM); Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012704
OSTI ID:
1456903
Report Number(s):
BNL-205792-2018-JAAM
Journal Information:
Scientific Reports, Vol. 8, Issue 1; ISSN 2045-2322
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 35 works
Citation information provided by
Web of Science

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Chemical diffusion in molybdenum disulphide journal April 2007
Point Defects and Grain Boundaries in Rotationally Commensurate MoS 2 on Epitaxial Graphene journal March 2016
Environment-Controlled Dislocation Migration and Superplasticity in Monolayer MoS 2 journal April 2015
Electrical and Optical Characterization of MoS 2 with Sulfur Vacancy Passivation by Treatment with Alkanethiol Molecules journal July 2015
Structural Characterization and Thermal Stability of MoS 2 Intercalation Compounds journal August 1998
Preparation and Characterization of a New Crystalline Form of Molybdenum Disulfide journal July 1957
Bandgap, Mid-Gap States, and Gating Effects in MoS 2 journal July 2014
Coherent Atomic and Electronic Heterostructures of Single-Layer MoS2 journal July 2012
Defect-Dominated Doping and Contact Resistance in MoS 2 journal February 2014
The chemistry of two-dimensional layered transition metal dichalcogenide nanosheets journal April 2013
Exploring atomic defects in molybdenum disulphide monolayers journal February 2015
Bandgap tunability at single-layer molybdenum disulphide grain boundaries journal February 2015
Single-layer MoS2 transistors journal January 2011
Electronics and optoelectronics of two-dimensional transition metal dichalcogenides journal November 2012
Ultrasensitive photodetectors based on monolayer MoS2 journal June 2013
Atomic mechanism of the semiconducting-to-metallic phase transition in single-layered MoS2 journal April 2014
Controlled Scalable Synthesis of Uniform, High-Quality Monolayer and Few-layer MoS2 Films journal May 2013
Inter-Layer Coupling Induced Valence Band Edge Shift in Mono- to Few-Layer MoS2 journal January 2017
High-sensitivity quantitative Kelvin probe microscopy by noncontact ultra-high-vacuum atomic force microscopy journal July 1999
Vacuum ultraviolet radiation effects on two-dimensional MoS 2 field-effect transistors journal February 2017
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Effect of contaminations and surface preparation on the work function of single layer MoS 2 journal January 2014
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The Nature of Electronic States in Atomically Thin MoS2 Field-Effect Transistors text January 2012
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Direct imaging of the band profile in single layer ${\small MoS_2}$ on graphite: quasiparticle energy gap, metallic edge states and edge band bending text January 2014
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Cited By (6)

Theoretical Analysis of Surface Active Sites in Defective 2H and 1T′ MoS 2 Polymorphs for Hydrogen Evolution Reaction: Quantifying the Total Activity of Point Defects journal January 2020
Imaging Nanoscale Inhomogeneities and Edge Delamination in As‐Grown MoS 2 Using Tip‐Enhanced Photoluminescence journal May 2019
Local electrical characterization of two-dimensional materials with functional atomic force microscopy journal January 2019
In situ high temperature atomic level dynamics of large inversion domain formations in monolayer MoS 2 journal January 2019
In situ work-function measurement during chemical transformation of MoS 2 to MoO 3 by ambient-pressure x-ray photoelectron spectroscopy journal February 2020
Imaging Nanoscale Inhomogeneities and Edge Delamination in As-Grown MoS2 Using Tip-Enhanced Photoluminescence text January 2019