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Title: Raman shifts in electron-irradiated monolayer MoS2

Journal Article · · ACS Nano
 [1];  [1];  [2];  [1];  [3];  [1];  [1];  [1];  [3];  [1]
  1. Univ. of Pennsylvania, Philadelphia, PA (United States)
  2. Rensselaer Polytechnic Inst., Troy, NY (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Rensselaer Polytechnic Inst., Troy, NY (United States)

Here, we report how the presence of electron-beam-induced sulfur vacancies affects first-order Raman modes and correlate the effects with the evolution of the in situ transmission-electron microscopy (TEM) two-terminal conductivity of monolayer MoS2 under electron irradiation. We observe a redshift in the E Raman peak and a less pronounced blueshift in the A'1 peak with increasing electron dose. Using energy-dispersive X-ray spectroscopy (EDS), we show that irradiation causes partial removal of sulfur and correlate the dependence of the Raman peak shifts with S vacancy density (a few %), which is confirmed by first-principles density functional theory calculations. In situ device current measurements show exponential decrease in channel current upon irradiation. Our analysis demonstrates that the observed frequency shifts are intrinsic properties of the defective systems and that Raman spectroscopy can be used as a quantitative diagnostic tool to characterize MoS2-based transport channels.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1250414
Journal Information:
ACS Nano, Vol. 10, Issue 4; ISSN 1936-0851
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 287 works
Citation information provided by
Web of Science

References (43)

Electronics and optoelectronics of two-dimensional transition metal dichalcogenides journal November 2012
Emerging Device Applications for Semiconducting Two-Dimensional Transition Metal Dichalcogenides journal January 2014
Influence of quantum confinement on the electronic structure of the transition metal sulfide T S 2 journal June 2011
Atomically Thin MoS2 A New Direct-Gap Semiconductor journal September 2010
Single-layer MoS2 transistors journal January 2011
Emerging Photoluminescence in Monolayer MoS2 journal April 2010
Electroluminescence in Single Layer MoS2 journal March 2013
Synthesis of Large-Area MoS2 Atomic Layers with Chemical Vapor Deposition journal March 2012
Integrated Circuits Based on Bilayer MoS2 Transistors journal January 2012
Integrated Circuits and Logic Operations Based on Single-Layer MoS 2 journal November 2011
DNA Base Detection Using a Single-Layer MoS 2 journal July 2014
Intrinsic Structural Defects in Monolayer Molybdenum Disulfide journal May 2013
Defect-Dominated Doping and Contact Resistance in MoS 2 journal February 2014
Impact of intrinsic atomic defects on the electronic structure of MoS 2 monolayers journal August 2014
Seeded growth of highly crystalline molybdenum disulphide monolayers at controlled locations journal January 2015
Sub-10 nm Device Fabrication in a Transmission Electron Microscope journal May 2007
First-principles Raman spectra of MoS2, WS2 and their heterostructures journal January 2014
Anomalous Lattice Vibrations of Single- and Few-Layer MoS 2 journal March 2010
From Bulk to Monolayer MoS2: Evolution of Raman Scattering journal January 2012
Two-Dimensional Transition Metal Dichalcogenides under Electron Irradiation: Defect Production and Doping journal July 2012
From point to extended defects in two-dimensional MoS 2 : Evolution of atomic structure under electron irradiation journal July 2013
Accurate Measurement of Electron Beam Induced Displacement Cross Sections for Single-Layer Graphene journal May 2012
Exploring atomic defects in molybdenum disulphide monolayers journal February 2015
Effect of disorder on Raman scattering of single-layer Mo S 2 journal May 2015
The origin of specimen contamination in the electron microscope journal April 1953
The sources of electron-induced contamination in kinetic vacuum systems journal January 1954
Correlations between ionization radiation damage and charging effects in transmission electron microscopy journal October 1995
Symmetry-dependent phonon renormalization in monolayer MoS 2 transistor journal April 2012
Atomic Healing of Defects in Transition Metal Dichalcogenides journal April 2015
Influence of Stoichiometry on the Optical and Electrical Properties of Chemical Vapor Deposition Derived MoS 2 journal September 2014
Hopping transport through defect-induced localized states in molybdenum disulphide journal October 2013
Defect-induced conductivity anisotropy in MoS 2 monolayers journal December 2013
Vapour phase growth and grain boundary structure of molybdenum disulphide atomic layers journal June 2013
Baseline correction using adaptive iteratively reweighted penalized least squares journal January 2010
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
Interlayer Breathing and Shear Modes in Few-Trilayer MoS 2 and WSe 2 journal February 2013
Probing the Interlayer Coupling of Twisted Bilayer MoS 2 Using Photoluminescence Spectroscopy journal September 2014
Phonons in single-layer and few-layer MoS 2 and WS 2 journal October 2011
Low-Frequency Raman Fingerprints of Two-Dimensional Metal Dichalcogenide Layer Stacking Configurations journal May 2015
Special points for Brillouin-zone integrations journal June 1976
First-principles calculations of the ferroelastic transition between rutile-type and CaCl 2 -type SiO 2 at high pressures journal October 2008
Low-Frequency Interlayer Breathing Modes in Few-Layer Black Phosphorus journal May 2015
A Supernodal Approach to Sparse Partial Pivoting journal January 1999

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Polarized Raman spectroscopy to elucidate the texture of synthesized MoS 2 journal January 2019
Electrical and geometrical tuning of MoS 2 field effect transistors via direct nanopatterning journal January 2019
Metal–organic framework-derived hierarchical MoS 2 /CoS 2 nanotube arrays as pH-universal electrocatalysts for efficient hydrogen evolution journal January 2019
Atomic Defects in Two-Dimensional Materials: From Single-Atom Spectroscopy to Functionalities in Opto-/Electronics, Nanomagnetism, and Catalysis journal March 2017
Effect of vacancies on the structural and electronic properties of Ti 2 CO 2 journal January 2019
Efficient Mechanochemical Preparation of Graphene-Like Molybdenum Disulfide and Graphene-Based Composite Electrocatalysts for Hydrogen Evolution Reaction journal April 2019
Hole Injection and Rectifying Heterojunction Photodiodes through Vacancy Engineering in MoS 2 journal April 2019
Density functional theory study of electronic structure of defects and the role on the strain relaxation behavior of MoS2 bilayer structures journal March 2018
Uncovering edge states and electrical inhomogeneity in MoS 2 field-effect transistors journal July 2016
Influence of impurities on structural, electronic and optical properties of graphene-like nano-layers MoSe 2 journal December 2019
Reversible alternation between bipolar and unipolar resistive switching in Ag/MoS 2 /Au structure for multilevel flexible memory journal January 2018
Solution-processable 2D semiconductors for high-performance large-area electronics journal October 2018
Irradiation of Transition Metal Dichalcogenides Using a Focused Ion Beam: Controlled Single‐Atom Defect Creation journal August 2019
Enhanced Photocurrent Generation in Proton‐Irradiated “Giant” CdSe/CdS Core/Shell Quantum Dots journal September 2019
Recent Progress on Irradiation-Induced Defect Engineering of Two-Dimensional 2H-MoS2 Few Layers journal February 2019
Strong edge-induced ferromagnetism in sputtered MoS 2 film treated by post-annealing journal November 2019
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Laser Synthesis, Processing, and Spectroscopy of Atomically-Thin Two Dimensional Materials book January 2018
Controlling neutral and charged excitons in MoS 2 with defects journal January 2020
Patterning metal contacts on monolayer MoS2 with vanishing Schottky barriers using thermal nanolithography journal January 2019
Tuning Transport and Photoelectric Performance of Monolayer MoS 2 Device by E-Beam Irradiation journal May 2018
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Improved luminescence properties of MoS 2 monolayers grown via MOCVD: role of pre-treatment and growth parameters journal May 2018
Cathodoluminescence enhancement and quenching in type-I van der Waals heterostructures: Cleanliness of the interfaces and defect creation journal November 2019
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Carbon vacancies in Ti 2 CT 2 MXenes: defects or a new opportunity? journal January 2017
Defect‐Engineered Atomically Thin MoS 2 Homogeneous Electronics for Logic Inverters journal November 2019
Evolution of Metastable Defects and Its Effect on the Electronic Properties of MoS2 Films journal April 2018
Reversible crystalline-to-amorphous phase transformation in monolayer MoS 2 under grazing ion irradiation journal January 2020
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