Excitation and characterization of image potential state electrons on quasi-free-standing graphene
Abstract
We investigate the band structure of image potential states in quasi-free-standing graphene (QFG) monolayer islands using angle-resolved two-photon-photoemission spectroscopy. Direct probing by low-energy electron diffraction shows that QFG is formed following oxygen intercalation into the graphene-Ir(111) interface. Despite the apparent decoupling of the monolayer graphene from the Ir substrate, we find that the binding energy of the n = 1 image potential state on these QFG islands increases by 0.17 eV, as compared to the original Gr/Ir(111) interface. We use calculations based on density-functional theory to construct an empirical, one-dimensional potential that quantitatively reproduces the image potential state binding energy and links the changes in the interface structure to the shift in energy. Specifically, two factors contribute comparably to this energy shift: a deeper potential well arising from the presence of intercalated oxygen adatoms and a wider potential well associated with the increase in the graphene-Ir distance. While image potential states have not been observed previously on QFG by photoemission, our paper now demonstrates that they may be strongly excited in a well-defined QFG system produced by oxygen intercalation. Finally, this opens an opportunity for studying the surface electron dynamics in QFG systems, beyond those found in typical nonintercalated graphene-on-substratemore »
- Authors:
-
- Columbia Univ., New York, NY (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1433982
- Alternate Identifier(s):
- OSTI ID: 1432421
- Report Number(s):
- BNL-203522-2018-JAAM
Journal ID: ISSN 2469-9950; PRBMDO; TRN: US1802384
- Grant/Contract Number:
- SC0012704; FG02-90ER14104
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 97; Journal Issue: 16; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
Citation Formats
Lin, Yi, Li, Yunzhe, Sadowski, Jerzy T., Jin, Wencan, Dadap, Jerry I., Hybertsen, Mark S., and Osgood, Richard M. Excitation and characterization of image potential state electrons on quasi-free-standing graphene. United States: N. p., 2018.
Web. doi:10.1103/PhysRevB.97.165413.
Lin, Yi, Li, Yunzhe, Sadowski, Jerzy T., Jin, Wencan, Dadap, Jerry I., Hybertsen, Mark S., & Osgood, Richard M. Excitation and characterization of image potential state electrons on quasi-free-standing graphene. United States. https://doi.org/10.1103/PhysRevB.97.165413
Lin, Yi, Li, Yunzhe, Sadowski, Jerzy T., Jin, Wencan, Dadap, Jerry I., Hybertsen, Mark S., and Osgood, Richard M. Mon .
"Excitation and characterization of image potential state electrons on quasi-free-standing graphene". United States. https://doi.org/10.1103/PhysRevB.97.165413. https://www.osti.gov/servlets/purl/1433982.
@article{osti_1433982,
title = {Excitation and characterization of image potential state electrons on quasi-free-standing graphene},
author = {Lin, Yi and Li, Yunzhe and Sadowski, Jerzy T. and Jin, Wencan and Dadap, Jerry I. and Hybertsen, Mark S. and Osgood, Richard M.},
abstractNote = {We investigate the band structure of image potential states in quasi-free-standing graphene (QFG) monolayer islands using angle-resolved two-photon-photoemission spectroscopy. Direct probing by low-energy electron diffraction shows that QFG is formed following oxygen intercalation into the graphene-Ir(111) interface. Despite the apparent decoupling of the monolayer graphene from the Ir substrate, we find that the binding energy of the n = 1 image potential state on these QFG islands increases by 0.17 eV, as compared to the original Gr/Ir(111) interface. We use calculations based on density-functional theory to construct an empirical, one-dimensional potential that quantitatively reproduces the image potential state binding energy and links the changes in the interface structure to the shift in energy. Specifically, two factors contribute comparably to this energy shift: a deeper potential well arising from the presence of intercalated oxygen adatoms and a wider potential well associated with the increase in the graphene-Ir distance. While image potential states have not been observed previously on QFG by photoemission, our paper now demonstrates that they may be strongly excited in a well-defined QFG system produced by oxygen intercalation. Finally, this opens an opportunity for studying the surface electron dynamics in QFG systems, beyond those found in typical nonintercalated graphene-on-substrate systems.},
doi = {10.1103/PhysRevB.97.165413},
journal = {Physical Review B},
number = 16,
volume = 97,
place = {United States},
year = {2018},
month = {4}
}
Web of Science
Figures / Tables:

Works referenced in this record:
One-dimensional potential for image-potential states on graphene
journal, February 2014
- de Andres, P. L.; Echenique, P. M.; Niesner, D.
- New Journal of Physics, Vol. 16, Issue 2
Surface core level shifts of clean and oxygen covered Ir(111)
journal, June 2009
- Bianchi, M.; Cassese, D.; Cavallin, A.
- New Journal of Physics, Vol. 11, Issue 6
Image-potential states and energy-loss satellites in inverse photoemission spectra
journal, February 1983
- Johnson, P. D.; Smith, N. V.
- Physical Review B, Vol. 27, Issue 4
Quasi-elastic scattering of electrons in image-potential states
journal, January 2007
- Fauster, Thomas; Weinelt, Martin; Höfer, Ulrich
- Progress in Surface Science, Vol. 82, Issue 4-6
Mechanical Decoupling of Graphene from Ru(0001) by Interfacial Reaction with Oxygen
journal, March 2013
- Sutter, Peter; Albrecht, Peter; Tong, Xiao
- The Journal of Physical Chemistry C, Vol. 117, Issue 12
Electronic structure and imaging contrast of graphene moiré on metals
journal, January 2013
- Voloshina, E. N.; Fertitta, E.; Garhofer, A.
- Scientific Reports, Vol. 3, Issue 1
Confinement of Dirac electrons in graphene quantum dots
journal, April 2014
- Jolie, Wouter; Craes, Fabian; Petrović, Marin
- Physical Review B, Vol. 89, Issue 15
Trapping surface electrons on graphene layers and islands
journal, February 2012
- Niesner, D.; Fauster, Th.; Dadap, J. I.
- Physical Review B, Vol. 85, Issue 8
Core level shifts of intercalated graphene
journal, November 2016
- Schröder, Ulrike A.; Petrović, Marin; Gerber, Timm
- 2D Materials, Vol. 4, Issue 1
Two-photon photoemission via image-potential states
journal, July 1985
- Giesen, K.; Hage, F.; Himpsel, F. J.
- Physical Review Letters, Vol. 55, Issue 3
Direct quantitative identification of the “surface trans-effect”
journal, January 2016
- Deimel, Peter S.; Bababrik, Reda M.; Wang, Bin
- Chemical Science, Vol. 7, Issue 9
Oxygen Switching of the Epitaxial Graphene–Metal Interaction
journal, October 2012
- Larciprete, Rosanna; Ulstrup, Søren; Lacovig, Paolo
- ACS Nano, Vol. 6, Issue 11
Two-photon photoemission from image-potential states of epitaxial graphene
journal, October 2015
- Gugel, Dieter; Niesner, Daniel; Eickhoff, Christian
- 2D Materials, Vol. 2, Issue 4
Li adsorption versus graphene intercalation on Ir(111): From quenching to restoration of the Ir surface state
journal, December 2015
- Pervan, P.; Lazić, P.; Petrović, M.
- Physical Review B, Vol. 92, Issue 24
An XPS investigation of the chemisorption of oxygen on the iridium (111) surface
journal, December 1976
- Zhdan, P. A.; Boreskov, G. K.; Boronin, A. I.
- Surface Science, Vol. 61, Issue 1
Low-energy electron diffraction structural analysis of the (2×2) oxygen overlayer on the iridium (111) surface
journal, January 1979
- Chan, C. -M.; Weinberg, W. H.
- The Journal of Chemical Physics, Vol. 71, Issue 7
Mapping Image Potential States on Graphene Quantum Dots
journal, July 2013
- Craes, Fabian; Runte, Sven; Klinkhammer, Jürgen
- Physical Review Letters, Vol. 111, Issue 5
Graphene on Ir(111): Physisorption with Chemical Modulation
journal, July 2011
- Busse, Carsten; Lazić, Predrag; Djemour, Rabie
- Physical Review Letters, Vol. 107, Issue 3
Nonequilibrium Band Mapping of Unoccupied Bulk States below the Vacuum Level by Two-Photon Photoemission
journal, July 2010
- Hao, Zhaofeng; Dadap, J. I.; Knox, K. R.
- Physical Review Letters, Vol. 105, Issue 1
Decay of electronic excitations at metal surfaces
journal, May 2004
- Echenique, P. M.; Berndt, R.; Chulkov, E. V.
- Surface Science Reports, Vol. 52, Issue 7-8
Interaction of oxygen with a clean Ir(111) surface
journal, June 1987
- Marinova, Ts. S.; Kostov, K. L.
- Surface Science, Vol. 185, Issue 1-2
Oxygen orders differently under graphene: new superstructures on Ir(111)
journal, January 2016
- Martínez-Galera, A. J.; Schröder, U. A.; Huttmann, F.
- Nanoscale, Vol. 8, Issue 4
Stability, structure, and electronic properties of chemisorbed oxygen and thin surface oxides on Ir(111)
journal, July 2008
- Zhang, Hong; Soon, Aloysius; Delley, Bernard
- Physical Review B, Vol. 78, Issue 4
Photoemission and density functional theory study of Ir(111); energy band gap mapping
journal, February 2010
- Pletikosić, I.; Kralj, M.; Šokčević, D.
- Journal of Physics: Condensed Matter, Vol. 22, Issue 13
Image potential states in graphene
journal, September 2009
- Silkin, V. M.; Zhao, J.; Guinea, F.
- Physical Review B, Vol. 80, Issue 12
Rashba Spin-Orbit Coupling in Image Potential States
journal, July 2015
- Tognolini, S.; Achilli, S.; Longetti, L.
- Physical Review Letters, Vol. 115, Issue 4
Semiempirical van der Waals correction to the density functional description of solids and molecular structures
journal, May 2006
- Ortmann, F.; Bechstedt, F.; Schmidt, W. G.
- Physical Review B, Vol. 73, Issue 20
Graphene on the Ir(111) surface: from van der Waals to strong bonding
journal, November 2010
- Brako, R.; Šokčević, D.; Lazić, P.
- New Journal of Physics, Vol. 12, Issue 11
The chemisorption of oxygen on the iridium (111) surface
journal, December 1976
- Ivanov, V. P.; Boreskov, G. K.; Savchenko, V. I.
- Surface Science, Vol. 61, Issue 1
Image-state electron scattering on flat and stepped metal surfaces
journal, April 2005
- Smadici, Serban; Osgood, Richard M.
- Physical Review B, Vol. 71, Issue 16
Ir(111) Surface State with Giant Rashba Splitting Persists under Graphene in Air
journal, February 2012
- Varykhalov, A.; Marchenko, D.; Scholz, M. R.
- Physical Review Letters, Vol. 108, Issue 6
Effective mass of image-potential states
journal, January 1987
- Giesen, K.; Hage, F.; Himpsel, F. J.
- Physical Review B, Vol. 35, Issue 3
Image-potential states of graphene on noble-metal surfaces
journal, November 2013
- Nobis, David; Potenz, Marco; Niesner, Daniel
- Physical Review B, Vol. 88, Issue 19
Sequential oxygen and alkali intercalation of epitaxial graphene on Ir(111): enhanced many-body effects and formation of pn -interfaces
journal, August 2014
- Ulstrup, Søren; Andersen, Mie; Bianchi, Marco
- 2D Materials, Vol. 1, Issue 2
Image-potential states and work function of graphene
journal, August 2014
- Niesner, Daniel; Fauster, Thomas
- Journal of Physics: Condensed Matter, Vol. 26, Issue 39
Quasi-Free-Standing Epitaxial Graphene on SiC Obtained by Hydrogen Intercalation
journal, December 2009
- Riedl, C.; Coletti, C.; Iwasaki, T.
- Physical Review Letters, Vol. 103, Issue 24
Image potential states as a quantum probe of graphene interfaces
journal, February 2010
- Bose, Sangita; Silkin, Vyacheslav M.; Ohmann, Robin
- New Journal of Physics, Vol. 12, Issue 2
Chemistry under Cover: Tuning Metal−Graphene Interaction by Reactive Intercalation
journal, June 2010
- Sutter, Peter; Sadowski, Jerzy T.; Sutter, Eli A.
- Journal of the American Chemical Society, Vol. 132, Issue 23
The changes in work function of group Ib and VIII metals on xenon adsorption, determined by field electron and photoelectron emission
journal, March 1974
- Nieuwenhuys, B. E.; Bouwman, R.; Sachtler, W. M. H.
- Thin Solid Films, Vol. 21, Issue 1
Surface oxides of Ir(111) prepared by gas-phase oxygen atoms
journal, December 2012
- Chung, Wen-Hung; Tsai, Dah-Shyang; Fan, Liang-Jen
- Surface Science, Vol. 606, Issue 23-24
The existence and detection of Rydberg states at surfaces
journal, May 1978
- Echenique, P. M.; Pendry, J. B.
- Journal of Physics C: Solid State Physics, Vol. 11, Issue 10
Model potential for the description of metal/organic interface states
journal, April 2017
- Armbrust, Nico; Schiller, Frederik; Güdde, Jens
- Scientific Reports, Vol. 7, Issue 1
The mechanism of caesium intercalation of graphene
journal, November 2013
- Petrović, M.; Šrut Rakić, I.; Runte, S.
- Nature Communications, Vol. 4, Issue 1
Dirac Cones and Minigaps for Graphene on Ir(111)
journal, February 2009
- Pletikosić, I.; Kralj, M.; Pervan, P.
- Physical Review Letters, Vol. 102, Issue 5
Etching of graphene on Ir(111) with molecular oxygen
journal, January 2016
- Schröder, Ulrike A.; Grånäs, Elin; Gerber, Timm
- Carbon, Vol. 96
Oxygen Intercalation under Graphene on Ir(111): Energetics, Kinetics, and the Role of Graphene Edges
journal, October 2012
- Grånäs, Elin; Knudsen, Jan; Schröder, Ulrike A.
- ACS Nano, Vol. 6, Issue 11
Image potential states on metal surfaces: binding energies and wave functions
journal, September 1999
- Chulkov, E. V.; Silkin, V. M.; Echenique, P. M.
- Surface Science, Vol. 437, Issue 3
Oxidation of Graphene on Metals
journal, March 2010
- Starodub, Elena; Bartelt, Norman C.; McCarty, Kevin F.
- The Journal of Physical Chemistry C, Vol. 114, Issue 11
Image-Potential States Observed by Inverse Photoemission
journal, May 1984
- Dose, V.; Altmann, W.; Goldmann, A.
- Physical Review Letters, Vol. 52, Issue 21
Low-energy electron diffraction, Auger electron spectroscopy, and thermal desorption studies of chemisorbed CO and O2 on the (111) and stepped [6(111) × (100)] iridium surfaces
journal, July 1976
- Hagen, D. I.; Nieuwenhuys, B. E.; Rovida, G.
- Surface Science, Vol. 57, Issue 2
Graphene on Ir(111) characterized by angle-resolved photoemission
journal, August 2011
- Kralj, Marko; Pletikosić, Ivo; Petrović, Marin
- Physical Review B, Vol. 84, Issue 7
Adsorption and dissociation of O2 on Ir(111)
journal, June 2002
- Xu, Ye; Mavrikakis, Manos
- The Journal of Chemical Physics, Vol. 116, Issue 24
Time-Resolved Coherent Photoelectron Spectroscopy of Quantized Electronic States on Metal Surfaces
journal, September 1997
- Hofer, U.
- Science, Vol. 277, Issue 5331
Soft self-consistent pseudopotentials in a generalized eigenvalue formalism
journal, April 1990
- Vanderbilt, David
- Physical Review B, Vol. 41, Issue 11, p. 7892-7895
Ultrafast dynamics of electrons in image-potential states on clean and Xe-covered Cu(111)
journal, August 1996
- Wolf, M.; Knoesel, E.; Hertel, T.
- Physical Review B, Vol. 54, Issue 8
Band-gap engineering by Bi intercalation of graphene on Ir(111)
journal, April 2016
- Warmuth, Jonas; Bruix, Albert; Michiardi, Matteo
- Physical Review B, Vol. 93, Issue 16
Formation of image-potential states at the graphene/metal interface
journal, October 2015
- Armbrust, N.; Güdde, J.; Höfer, U.
- New Journal of Physics, Vol. 17, Issue 10
Image potential states in monolayer, bilayer, and trilayer epitaxial graphene studied with time- and angle-resolved two-photon photoemission spectroscopy
journal, April 2014
- Takahashi, Kazutoshi; Imamura, Masaki; Yamamoto, Isamu
- Physical Review B, Vol. 89, Issue 15
First principles methods using CASTEP
journal, January 2005
- Clark, Stewart J.; Segall, Matthew D.; Pickard, Chris J.
- Zeitschrift für Kristallographie - Crystalline Materials, Vol. 220, Issue 5/6
The quasi-free-standing nature of graphene on H-saturated SiC(0001)
journal, September 2011
- Speck, F.; Jobst, J.; Fromm, F.
- Applied Physics Letters, Vol. 99, Issue 12
Topography of the graphene/Ir(111) moiré studied by surface x-ray diffraction
journal, June 2015
- Jean, Fabien; Zhou, Tao; Blanc, Nils
- Physical Review B, Vol. 91, Issue 24
Restoring a nearly free-standing character of graphene on Ru(0001) by oxygen intercalation
journal, February 2016
- Voloshina, Elena; Berdunov, Nikolai; Dedkov, Yuriy
- Scientific Reports, Vol. 6, Issue 1
Understanding intercalation structures formed under graphene on Ir(111)
journal, October 2014
- Andersen, Mie; Hornekær, Liv; Hammer, Bjørk
- Physical Review B, Vol. 90, Issue 15
Works referencing / citing this record:
Observation of intercalation-driven zone folding in quasi-free-standing graphene energy bands
journal, January 2019
- Lin, Yi; Chen, Ge; Sadowski, Jerzy T.
- Physical Review B, Vol. 99, Issue 3
Figures / Tables found in this record: