Work Function Variations in Twisted Graphene Layers
Abstract
By combining optical imaging, Raman spectroscopy, kelvin probe force microscopy (KFPM), and photoemission electron microscopy (PEEM), we show that graphene’s layer orientation, as well as layer thickness, measurably changes the surface potential (Φ). Detailed mapping of variable-thickness, rotationally-faulted graphene films allows us to correlate Φ with specific morphological features. Using KPFM and PEEM we measure ΔΦ up to 39 mV for layers with different twist angles, while ΔΦ ranges from 36–129 mV for different layer thicknesses. The surface potential between different twist angles or layer thicknesses is measured at the KPFM instrument resolution of ≤ 200 nm. The PEEM measured work function of 4.4 eV for graphene is consistent with doping levels on the order of 1012cm-2. Here, we find that Φ scales linearly with Raman G-peak wavenumber shift (slope = 22.2 mV/cm-1) for all layers and twist angles, which is consistent with doping-dependent changes to graphene’s Fermi energy in the ‘high’ doping limit. Our results here emphasize that layer orientation is equally important as layer thickness when designing multilayer two-dimensional systems where surface potential is considered.
- Authors:
-
- Naval Research Lab. (NRL), Washington, DC (United States). Electronics Science and Technology Division
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Center for Integrated Nanotechnologies
- Publication Date:
- Research Org.:
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); US Department of the Navy, Office of Naval Research (ONR)
- OSTI Identifier:
- 1426807
- Report Number(s):
- SAND-2018-1772J
Journal ID: ISSN 2045-2322; 660738
- Grant/Contract Number:
- AC04-94AL85000; NA0003525
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Scientific Reports
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2045-2322
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Robinson, Jeremy T., Culbertson, James, Berg, Morgann, and Ohta, Taisuke. Work Function Variations in Twisted Graphene Layers. United States: N. p., 2018.
Web. doi:10.1038/s41598-018-19631-4.
Robinson, Jeremy T., Culbertson, James, Berg, Morgann, & Ohta, Taisuke. Work Function Variations in Twisted Graphene Layers. United States. https://doi.org/10.1038/s41598-018-19631-4
Robinson, Jeremy T., Culbertson, James, Berg, Morgann, and Ohta, Taisuke. Wed .
"Work Function Variations in Twisted Graphene Layers". United States. https://doi.org/10.1038/s41598-018-19631-4. https://www.osti.gov/servlets/purl/1426807.
@article{osti_1426807,
title = {Work Function Variations in Twisted Graphene Layers},
author = {Robinson, Jeremy T. and Culbertson, James and Berg, Morgann and Ohta, Taisuke},
abstractNote = {By combining optical imaging, Raman spectroscopy, kelvin probe force microscopy (KFPM), and photoemission electron microscopy (PEEM), we show that graphene’s layer orientation, as well as layer thickness, measurably changes the surface potential (Φ). Detailed mapping of variable-thickness, rotationally-faulted graphene films allows us to correlate Φ with specific morphological features. Using KPFM and PEEM we measure ΔΦ up to 39 mV for layers with different twist angles, while ΔΦ ranges from 36–129 mV for different layer thicknesses. The surface potential between different twist angles or layer thicknesses is measured at the KPFM instrument resolution of ≤ 200 nm. The PEEM measured work function of 4.4 eV for graphene is consistent with doping levels on the order of 1012cm-2. Here, we find that Φ scales linearly with Raman G-peak wavenumber shift (slope = 22.2 mV/cm-1) for all layers and twist angles, which is consistent with doping-dependent changes to graphene’s Fermi energy in the ‘high’ doping limit. Our results here emphasize that layer orientation is equally important as layer thickness when designing multilayer two-dimensional systems where surface potential is considered.},
doi = {10.1038/s41598-018-19631-4},
journal = {Scientific Reports},
number = 1,
volume = 8,
place = {United States},
year = {Wed Jan 31 00:00:00 EST 2018},
month = {Wed Jan 31 00:00:00 EST 2018}
}
Web of Science
Works referenced in this record:
Variations in the work function of doped single- and few-layer graphene assessed by Kelvin probe force microscopy and density functional theory
journal, June 2011
- Ziegler, D.; Gava, P.; Güttinger, J.
- Physical Review B, Vol. 83, Issue 23
Determination of graphene work function and graphene-insulator-semiconductor band alignment by internal photoemission spectroscopy
journal, July 2012
- Yan, Rusen; Zhang, Qin; Li, Wei
- Applied Physics Letters, Vol. 101, Issue 2
Atomic Hole Doping of Graphene
journal, December 2008
- Gierz, Isabella; Riedl, Christian; Starke, Ulrich
- Nano Letters, Vol. 8, Issue 12
Work Function Engineering of Graphene Electrode via Chemical Doping
journal, March 2010
- Shi, Yumeng; Kim, Ki Kang; Reina, Alfonso
- ACS Nano, Vol. 4, Issue 5
The interlayer screening effect of graphene sheets investigated by Kelvin probe force microscopy
journal, November 2009
- Lee, N. J.; Yoo, J. W.; Choi, Y. J.
- Applied Physics Letters, Vol. 95, Issue 22
Stacking-Mode-Induced Reactivity Enhancement for Twisted Bilayer Graphene
journal, February 2016
- Ding, Yao; Peng, Qing; Gan, Lin
- Chemistry of Materials, Vol. 28, Issue 4
Large-Area Graphene Single Crystals Grown by Low-Pressure Chemical Vapor Deposition of Methane on Copper
journal, March 2011
- Li, Xuesong; Magnuson, Carl W.; Venugopal, Archana
- Journal of the American Chemical Society, Vol. 133, Issue 9, p. 2816-2819
Interlayer screening effect in graphene multilayers with and stacking
journal, March 2010
- Koshino, Mikito
- Physical Review B, Vol. 81, Issue 12
Experimental Determination of the Ionization Energies of MoSe 2 , WS 2 , and MoS 2 on SiO 2 Using Photoemission Electron Microscopy
journal, July 2017
- Keyshar, Kunttal; Berg, Morgann; Zhang, Xiang
- ACS Nano, Vol. 11, Issue 8
Open loop Kelvin probe force microscopy with single and multi-frequency excitation
journal, October 2013
- Collins, L.; Kilpatrick, J. I.; Weber, S. A. L.
- Nanotechnology, Vol. 24, Issue 47
Increased Work Function in Few-Layer Graphene Sheets via Metal Chloride Doping
journal, July 2012
- Kwon, Ki Chang; Choi, Kyoung Soon; Kim, Soo Young
- Advanced Functional Materials, Vol. 22, Issue 22
Growth from below: bilayer graphene on copper by chemical vapor deposition
journal, September 2012
- Nie, Shu; Wu, Wei; Xing, Shirui
- New Journal of Physics, Vol. 14, Issue 9
Corrugation in Exfoliated Graphene: An Electron Microscopy and Diffraction Study
journal, July 2010
- Locatelli, Andrea; Knox, Kevin R.; Cvetko, Dean
- ACS Nano, Vol. 4, Issue 8
Electronic Properties of Graphene Encapsulated with Different Two-Dimensional Atomic Crystals
journal, May 2014
- Kretinin, A. V.; Cao, Y.; Tu, J. S.
- Nano Letters, Vol. 14, Issue 6
Evidence for Interlayer Coupling and Moiré Periodic Potentials in Twisted Bilayer Graphene
journal, November 2012
- Ohta, Taisuke; Robinson, Jeremy T.; Feibelman, Peter J.
- Physical Review Letters, Vol. 109, Issue 18
Tuning the Graphene Work Function by Electric Field Effect
journal, October 2009
- Yu, Young-Jun; Zhao, Yue; Ryu, Sunmin
- Nano Letters, Vol. 9, Issue 10, p. 3430-3434
Stacking-Dependent Optical Conductivity of Bilayer Graphene
journal, June 2010
- Wang, Yingying; Ni, Zhenhua; Liu, Lei
- ACS Nano, Vol. 4, Issue 7
Layer dependence of the electronic band alignment of few-layer on measured using photoemission electron microscopy
journal, June 2017
- Berg, Morgann; Keyshar, Kunttal; Bilgin, Ismail
- Physical Review B, Vol. 95, Issue 23
Chiral atomically thin films
journal, February 2016
- Kim, Cheol-Joo; Sánchez-Castillo, A.; Ziegler, Zack
- Nature Nanotechnology, Vol. 11, Issue 6
Angle-Resolved Raman Imaging of Interlayer Rotations and Interactions in Twisted Bilayer Graphene
journal, May 2012
- Havener, Robin W.; Zhuang, Houlong; Brown, Lola
- Nano Letters, Vol. 12, Issue 6
Asymmetric Growth of Bilayer Graphene on Copper Enclosures Using Low-Pressure Chemical Vapor Deposition
journal, May 2014
- Fang, Wenjing; Hsu, Allen L.; Song, Yi
- ACS Nano, Vol. 8, Issue 6
Raman Spectroscopy Study of Rotated Double-Layer Graphene: Misorientation-Angle Dependence of Electronic Structure
journal, June 2012
- Kim, Kwanpyo; Coh, Sinisa; Tan, Liang Z.
- Physical Review Letters, Vol. 108, Issue 24
Surface Potentials and Layer Charge Distributions in Few-Layer Graphene Films
journal, January 2009
- Datta, Sujit S.; Strachan, Douglas R.; Mele, E. J.
- Nano Letters, Vol. 9, Issue 1
Observation of Anomalous Phonon Softening in Bilayer Graphene
journal, September 2008
- Yan, Jun; Henriksen, Erik A.; Kim, Philip
- Physical Review Letters, Vol. 101, Issue 13
Quantum Hall effect in Bernal stacked and twisted bilayer graphene grown on Cu by chemical vapor deposition
journal, May 2012
- Fallahazad, Babak; Hao, Yufeng; Lee, Kayoung
- Physical Review B, Vol. 85, Issue 20
Raman Spectrum of Graphene and Graphene Layers
journal, October 2006
- Ferrari, A. C.; Meyer, J. C.; Scardaci, V.
- Physical Review Letters, Vol. 97, Issue 18, Article No. 187401
Electric Field Effect Tuning of Electron-Phonon Coupling in Graphene
journal, April 2007
- Yan, Jun; Zhang, Yuanbo; Kim, Philip
- Physical Review Letters, Vol. 98, Issue 16
Atmospheric Oxygen Binding and Hole Doping in Deformed Graphene on a SiO2 Substrate
journal, December 2010
- Ryu, Sunmin; Liu, Li; Berciaud, Stephane
- Nano Letters, Vol. 10, Issue 12, p. 4944-4951
Local work function measurements of epitaxial graphene
journal, September 2008
- Filleter, T.; Emtsev, K. V.; Seyller, Th.
- Applied Physics Letters, Vol. 93, Issue 13
Doping-Induced Tunable Wettability and Adhesion of Graphene
journal, June 2016
- Ashraf, Ali; Wu, Yanbin; Wang, Michael Cai
- Nano Letters, Vol. 16, Issue 7
Electronic Hybridization of Large-Area Stacked Graphene Films
journal, December 2012
- Robinson, Jeremy T.; Schmucker, Scott W.; Diaconescu, C. Bogdan
- ACS Nano, Vol. 7, Issue 1
Effective doping of single-layer graphene from underlying substrates
journal, March 2009
- Shi, Yumeng; Dong, Xiaochen; Chen, Peng
- Physical Review B, Vol. 79, Issue 11
Standardization of surface potential measurements of graphene domains
journal, September 2013
- Panchal, Vishal; Pearce, Ruth; Yakimova, Rositza
- Scientific Reports, Vol. 3, Issue 1
Carrier type inversion in quasi-free standing graphene: studies of local electronic and structural properties
journal, June 2015
- Melios, Christos; Panchal, Vishal; Giusca, Cristina E.
- Scientific Reports, Vol. 5, Issue 1
Moiré butterflies in twisted bilayer graphene
journal, July 2011
- Bistritzer, R.; MacDonald, A. H.
- Physical Review B, Vol. 84, Issue 3
Atomic Hole Doping of Graphene
text, January 2008
- Gierz, Isabella; Riedl, Christian; Starke, Ulrich
- arXiv
Single Layer Behavior and Its Breakdown in Twisted Graphene Layers
text, January 2010
- Luican, A.; Li, Guohong; Reina, A.
- arXiv
Quantum Hall Effect, Screening and Layer-Polarized Insulating States in Twisted Bilayer Graphene
text, January 2011
- Sanchez-Yamagishi, Javier D.; Taychatanapat, Thiti; Watanabe, Kenji
- arXiv
Growth from Below: Bilayer Graphene on Copper by Chemical Vapor Deposition
text, January 2012
- Nie, Shu; Wu, Wei; Xing, Shirui
- arXiv
Quantum Hall Effect in Bernal Stacked and Twisted Bilayer Graphene Grown on Cu by Chemical Vapor Deposition
text, January 2012
- Fallahazad, Babak; Hao, Yufeng; Lee, Kayoung
- arXiv
Electronic Hybridization of Large-Area Stacked Graphene Films
text, January 2013
- Robinson, Jeremy T.; Schmucker, Scott W.; Diaconescu, C. Bogdan
- arXiv
Increased Work Function in Few-Layer Graphene Sheets via Metal Chloride Doping
journal, July 2012
- Kwon, Ki Chang; Choi, Kyoung Soon; Kim, Soo Young
- Advanced Functional Materials, Vol. 22, Issue 22
Stacking-Mode-Induced Reactivity Enhancement for Twisted Bilayer Graphene
journal, February 2016
- Ding, Yao; Peng, Qing; Gan, Lin
- Chemistry of Materials, Vol. 28, Issue 4
Large-Area Graphene Single Crystals Grown by Low-Pressure Chemical Vapor Deposition of Methane on Copper
journal, March 2011
- Li, Xuesong; Magnuson, Carl W.; Venugopal, Archana
- Journal of the American Chemical Society, Vol. 133, Issue 9, p. 2816-2819
Angle-Resolved Raman Imaging of Interlayer Rotations and Interactions in Twisted Bilayer Graphene
journal, May 2012
- Havener, Robin W.; Zhuang, Houlong; Brown, Lola
- Nano Letters, Vol. 12, Issue 6
Surface Potentials and Layer Charge Distributions in Few-Layer Graphene Films
journal, January 2009
- Datta, Sujit S.; Strachan, Douglas R.; Mele, E. J.
- Nano Letters, Vol. 9, Issue 1
Stacking-Dependent Optical Conductivity of Bilayer Graphene
journal, June 2010
- Wang, Yingying; Ni, Zhenhua; Liu, Lei
- ACS Nano, Vol. 4, Issue 7
Work Function Engineering of Graphene Electrode via Chemical Doping
journal, March 2010
- Shi, Yumeng; Kim, Ki Kang; Reina, Alfonso
- ACS Nano, Vol. 4, Issue 5
Corrugation in Exfoliated Graphene: An Electron Microscopy and Diffraction Study
journal, July 2010
- Locatelli, Andrea; Knox, Kevin R.; Cvetko, Dean
- ACS Nano, Vol. 4, Issue 8
Electronic Hybridization of Large-Area Stacked Graphene Films
journal, December 2012
- Robinson, Jeremy T.; Schmucker, Scott W.; Diaconescu, C. Bogdan
- ACS Nano, Vol. 7, Issue 1
Asymmetric Growth of Bilayer Graphene on Copper Enclosures Using Low-Pressure Chemical Vapor Deposition
journal, May 2014
- Fang, Wenjing; Hsu, Allen L.; Song, Yi
- ACS Nano, Vol. 8, Issue 6
Chiral atomically thin films
journal, February 2016
- Kim, Cheol-Joo; Sánchez-Castillo, A.; Ziegler, Zack
- Nature Nanotechnology, Vol. 11, Issue 6
Carrier type inversion in quasi-free standing graphene: studies of local electronic and structural properties
journal, June 2015
- Melios, Christos; Panchal, Vishal; Giusca, Cristina E.
- Scientific Reports, Vol. 5, Issue 1
The interlayer screening effect of graphene sheets investigated by Kelvin probe force microscopy
journal, November 2009
- Lee, N. J.; Yoo, J. W.; Choi, Y. J.
- Applied Physics Letters, Vol. 95, Issue 22
Determination of graphene work function and graphene-insulator-semiconductor band alignment by internal photoemission spectroscopy
journal, July 2012
- Yan, Rusen; Zhang, Qin; Li, Wei
- Applied Physics Letters, Vol. 101, Issue 2
Single-Layer Behavior and Its Breakdown in Twisted Graphene Layers
journal, March 2011
- Luican, A.; Li, Guohong; Reina, A.
- Physical Review Letters, Vol. 106, Issue 12
Quantum Hall Effect, Screening, and Layer-Polarized Insulating States in Twisted Bilayer Graphene
journal, February 2012
- Sanchez-Yamagishi, Javier D.; Taychatanapat, Thiti; Watanabe, Kenji
- Physical Review Letters, Vol. 108, Issue 7
Interlayer Interaction and Electronic Screening in Multilayer Graphene Investigated with Angle-Resolved Photoemission Spectroscopy
journal, May 2007
- Ohta, Taisuke; Bostwick, Aaron; McChesney, J. L.
- Physical Review Letters, Vol. 98, Issue 20
Observation of Anomalous Phonon Softening in Bilayer Graphene
text, January 2007
- Yan, Jun; Henriksen, Erik A.; Kim, Philip
- arXiv
Atomic Hole Doping of Graphene
text, January 2008
- Gierz, Isabella; Riedl, Christian; Starke, Ulrich
- arXiv
Growth from Below: Bilayer Graphene on Copper by Chemical Vapor Deposition
text, January 2012
- Nie, Shu; Wu, Wei; Xing, Shirui
- arXiv
Quantum Hall Effect in Bernal Stacked and Twisted Bilayer Graphene Grown on Cu by Chemical Vapor Deposition
text, January 2012
- Fallahazad, Babak; Hao, Yufeng; Lee, Kayoung
- arXiv
Electronic Properties of Graphene Encapsulated with Different Two-Dimensional Atomic Crystals
text, January 2014
- Kretinin, A. V.; Cao, Y.; Tu, J. S.
- arXiv
Electric Field Effect Tuning of Electron-Phonon Coupling in Graphene
text, January 2006
- Yan, Jun; Zhang, Yuanbo; Kim, Philip
- arXiv
Works referencing / citing this record:
Direct probing of imperfection-induced electrical degradation in millimeter-scale graphene on SiO 2 substrates
journal, August 2019
- Ma, Rui-Song; Ma, Jiajun; Yan, Jiahao
- 2D Materials, Vol. 6, Issue 4
Noninvasive Subsurface Electrical Probe for Encapsulated Layers in van der Waals Heterostructures
journal, December 2019
- Pandey, Mrityunjay; Soni, Radhika; Mathur, Avi
- Physical Review Applied, Vol. 12, Issue 6
A non-invasive sub-surface electrical probe to encapsulated layers in van der Waals heterostructures
text, January 2019
- Pandey, Mrityunjay; Soni, Radhika; Mathur, Avi
- arXiv