Raman shifts in electron-irradiated monolayer MoS2

Parkin, William M.; Balan, Adrian; Liang, Liangbo; Das, Paul Masih; Lamparski, Michael; Naylor, Carl H.; Rodríguez-Manzo, Julio A.; Johnson, A. T. Charlie; Meunier, Vincent; Drndic, Marija

doi:10.1021/acsnano.5b07388

Title: Raman shifts in electron-irradiated monolayer MoS₂

Abstract

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.

Authors:

Parkin, William M. ^[1]; Balan, Adrian ^[1]; Liang, Liangbo ^[2]; Das, Paul Masih ^[1]; Lamparski, Michael ^[3]; Naylor, Carl H. ^[1]; Rodríguez-Manzo, Julio A. ^[1]; Johnson, A. T. Charlie ^[1]; Meunier, Vincent ^[3]; Drndic, Marija ^[1]

Univ. of Pennsylvania, Philadelphia, PA (United States)
Rensselaer Polytechnic Inst., Troy, NY (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Rensselaer Polytechnic Inst., Troy, NY (United States)

Publication Date:: Mon Mar 21 00:00:00 EDT 2016

Research Org.:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC)

OSTI Identifier:: 1250414

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Journal Article: Accepted Manuscript

Journal Name:: ACS Nano

Additional Journal Information:: Journal Volume: 10; Journal Issue: 4; Journal ID: ISSN 1936-0851

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 77 NANOSCIENCE AND NANOTECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; MoS₂; two-dimensional material; Raman; in situ transmission electron microscopy; transition-metal dichalcogenide

Citation Formats


                    Parkin, William M., Balan, Adrian, Liang, Liangbo, Das, Paul Masih, Lamparski, Michael, Naylor, Carl H., Rodríguez-Manzo, Julio A., Johnson, A. T. Charlie, Meunier, Vincent, and Drndic, Marija. Raman shifts in electron-irradiated monolayer MoS2.  United States: N. p., 2016. 
        Web.  doi:10.1021/acsnano.5b07388.

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                    Parkin, William M., Balan, Adrian, Liang, Liangbo, Das, Paul Masih, Lamparski, Michael, Naylor, Carl H., Rodríguez-Manzo, Julio A., Johnson, A. T. Charlie, Meunier, Vincent, & Drndic, Marija. Raman shifts in electron-irradiated monolayer MoS2.  United States.  https://doi.org/10.1021/acsnano.5b07388

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                    Parkin, William M., Balan, Adrian, Liang, Liangbo, Das, Paul Masih, Lamparski, Michael, Naylor, Carl H., Rodríguez-Manzo, Julio A., Johnson, A. T. Charlie, Meunier, Vincent, and Drndic, Marija. 2016.  
        "Raman shifts in electron-irradiated monolayer MoS2".  United States.  https://doi.org/10.1021/acsnano.5b07388.  https://www.osti.gov/servlets/purl/1250414.

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@article{osti_1250414,

  title        = {Raman shifts in electron-irradiated monolayer MoS2},

  author       = {Parkin, William M. and Balan, Adrian and Liang, Liangbo and Das, Paul Masih and Lamparski, Michael and Naylor, Carl H. and Rodríguez-Manzo, Julio A. and Johnson, A. T. Charlie and Meunier, Vincent and Drndic, Marija},

  abstractNote = {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.},

  doi          = {10.1021/acsnano.5b07388},

  url          = {https://www.osti.gov/biblio/1250414},
  journal      = {ACS Nano},

  issn         = {1936-0851},

  number       = 4,

  volume       = 10,

  place        = {United States},

  year         = {Mon Mar 21 00:00:00 EDT 2016},

  month        = {Mon Mar 21 00:00:00 EDT 2016}

}

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journal, November 2019

Gao, Li; Liao, Qingliang; Zhang, Xiankun
Advanced Materials, Vol. 32, Issue 2
https://doi.org/10.1002/adma.201906646

Evolution of Metastable Defects and Its Effect on the Electronic Properties of MoS2 Films
journal, April 2018

Precner, M.; Polaković, T.; Qiao, Qiao
Scientific Reports, Vol. 8, Issue 1
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Reversible crystalline-to-amorphous phase transformation in monolayer MoS ₂ under grazing ion irradiation
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Electron radiation effects on the structural and electrical properties of MoS ₂ field effect transistors
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Laser-induced fabrication of nanoporous monolayer WS ₂ membranes
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Caveats in obtaining high-quality 2D materials and property characterization
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Low-defectiveness exfoliation of MoS2 nanoparticles and their embedment in hybrid light-emitting polymer nanofibers
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Suppression of the Shear Raman Mode in Defective Bilayer MoS2
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Designing artificial 2D crystals with site and size controlled quantum dots
journal, August 2017

Xie, Xuejun; Kang, Jiahao; Cao, Wei
Scientific Reports, Vol. 7, Issue 1
https://doi.org/10.1038/s41598-017-08776-3

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Title: Raman shifts in electron-irradiated monolayer MoS2

Abstract

Citation Formats

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

Photoresponsive behavior of electron-beam irradiated MoS 2 films journal, October 2018

Robust valley polarization of helium ion modified atomically thin MoS 2 journal, November 2017

Anomalous lattice vibrations of CVD-grown monolayer MoS 2 probed using linear polarized excitation light journal, January 2019

E’’ Raman Mode in Thermal Strain-Fractured CVD-MoS2 journal, November 2016

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

Changes in the Raman spectra of monolayer MoS 2 upon thermal annealing journal, August 2018

Hybrid nanobud-array structures (C 24 ) n /MoS 2 and (C 24 V) n /MoS 2 : two-dimensional half metallic and ferromagnetic materials journal, January 2018

Electrical reliability, multilevel data storage and mechanical stability of MoS 2 -PMMA nanocomposite-based non-volatile memory device journal, June 2017

Low-defectiveness exfoliation of MoS 2 nanoparticles and their embedment in hybrid light-emitting polymer nanofibers journal, January 2018

Photoluminescence Study of B-Trions in MoS 2 Monolayers with High Density of Defects journal, October 2018

Size-dependent Raman shift of semiconductor nanomaterials determined using bond number and strength journal, January 2017

Suppression of the shear Raman mode in defective bilayer MoS 2 journal, February 2019

Wafer‐Scale and Low‐Temperature Growth of 1T‐WS 2 Film for Efficient and Stable Hydrogen Evolution Reaction journal, January 2020

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

Role of oxygen adsorption in modification of optical and surface electronic properties of MoS 2 journal, April 2018

Improved luminescence properties of MoS 2 monolayers grown via MOCVD: role of pre-treatment and growth parameters journal, May 2018

Title: Raman shifts in electron-irradiated monolayer MoS₂

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 ${MoS}_{2}$ 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

Photoresponsive behavior of electron-beam irradiated MoS ₂ films
journal, October 2018

Robust valley polarization of helium ion modified atomically thin MoS ₂
journal, November 2017

Anomalous lattice vibrations of CVD-grown monolayer MoS ₂ probed using linear polarized excitation light
journal, January 2019

E’’ Raman Mode in Thermal Strain-Fractured CVD-MoS2
journal, November 2016

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

Changes in the Raman spectra of monolayer MoS ₂ upon thermal annealing
journal, August 2018

Hybrid nanobud-array structures (C ₂₄ ) _n /MoS ₂ and (C ₂₄ V) _n /MoS ₂ : two-dimensional half metallic and ferromagnetic materials
journal, January 2018

Electrical reliability, multilevel data storage and mechanical stability of MoS ₂ -PMMA nanocomposite-based non-volatile memory device
journal, June 2017

Low-defectiveness exfoliation of MoS ₂ nanoparticles and their embedment in hybrid light-emitting polymer nanofibers
journal, January 2018

Photoluminescence Study of B-Trions in MoS ₂ Monolayers with High Density of Defects
journal, October 2018

Size-dependent Raman shift of semiconductor nanomaterials determined using bond number and strength
journal, January 2017

Suppression of the shear Raman mode in defective bilayer MoS 2
journal, February 2019

Wafer‐Scale and Low‐Temperature Growth of 1T‐WS ₂ Film for Efficient and Stable Hydrogen Evolution Reaction
journal, January 2020

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

Role of oxygen adsorption in modification of optical and surface electronic properties of MoS ₂
journal, April 2018

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

Towards the evaluation of defects in MoS ₂ using cryogenic photoluminescence spectroscopy
journal, January 2020