Abstract
Graphene, a single layer of graphite, has recently attracted considerable attention owing to its remarkable electronic and structural properties and its possible applications in many emerging areas such as graphene-based electronic devices1. The charge carriers in graphene behave like massless Dirac fermions, and graphene shows ballistic charge transport, turning it into an ideal material for circuit fabrication2,3. However, graphene lacks a bandgap around the Fermi level, which is the defining concept for semiconductor materials and essential for controlling the conductivity by electronic means. Theory predicts that a tunable bandgap may be engineered by periodic modulations of the graphene lattice4,5,6, but experimental evidence for this is so far lacking. Here, we demonstrate the existence of a bandgap opening in graphene, induced by the patterned adsorption of atomic hydrogen onto the Moiré superlattice positions of graphene grown on an Ir(111) substrate.
This is a preview of subscription content, access via your institution
Relevant articles
Open Access articles citing this article.
-
Enhanced Removal of Diesel Oil Using New Magnetic Bentonite-Based Adsorbents Combined with Different Carbon Sources
Water, Air, & Soil Pollution Open Access 24 May 2022
-
Two-dimensional Stiefel-Whitney insulators in liganded Xenes
npj Computational Materials Open Access 10 January 2022
-
Deep Learning Method to Accelerate Discovery of Hybrid Polymer-Graphene Composites
Scientific Reports Open Access 23 July 2021
Access options
Subscribe to this journal
Receive 12 print issues and online access
$259.00 per year
only $21.58 per issue
Rent or buy this article
Get just this article for as long as you need it
$39.95
Prices may be subject to local taxes which are calculated during checkout




References
Geim, A. & Novoselov, K. The rise of graphene. Nature Mater. 6, 183–191 (2007).
Novoselov, K. et al. Two-dimensional gas of massless Dirac fermions in graphene. Nature 438, 197–200 (2005).
Hass, J. et al. Highly ordered graphene for two-dimensional electronics. Appl. Phys. Lett. 89, 143106 (2006).
Duplock, E. J., Scheffler, M. & Lindan, P. J. D. Hallmark of perfect graphene. Phys. Rev. Lett. 92, 225502 (2004).
Chernozatonskiǐ, L., Sorokin, P., Belova, E., Brüning, J. & Fedorov, A. Superlattices consisting of lines of adsorbed hydrogen atom pairs on graphene. JETP Lett. 85, 77–81 (2007).
Pedersen, T. et al. Graphene antidot lattices: Designed defects and spin qubits. Phys. Rev. Lett. 100, 136804 (2008).
Giovannetti, G., Khomyakov, P. A., Brocks, G., Kelly, P. J. & van den Brink, J. Substrate-induced band gap in graphene on hexagonal boron nitride: Ab initio density functional calculations. Phys. Rev. B 76, 073103 (2007).
Son, Y., Cohen, M. & Louie, S. Energy gaps in graphene nanoribbons. Phys. Rev. Lett. 97, 1–4 (2006).
Zhou, S. Y. et al. Origin of the energy bandgap in epitaxial graphene—reply. Nature Mater. 7, 259–260 (2008).
Rotenberg, E. et al. Origin of the energy bandgap in epitaxial graphene. Nature Mater. 7, 258–259 (2008).
Berger, C. Electronic confinement and coherence in patterned epitaxial graphene. Science 312, 1191–1196 (2006).
Han, M. Y., Oezyilmaz, B., Zhang, Y. & Kim, P. Energy band-gap engineering of graphene nanoribbons. Phys. Rev. Lett. 98, 206805 (2007).
Barone, V., Hod, O. & Scuseria, G. E. Electronic structure and stability of semiconducting graphene nanoribbons. Nano Lett. 6, 2748–2754 (2006).
Lu, Y. H. et al. Effects of edge passivation by hydrogen on electronic structure of armchair graphene nanoribbon and band gap engineering. Appl. Phys. Lett. 94, 122111 (2009).
Vanevic, M., Stojanovic, V. M. & Kindermann, M. Character of electronic states in graphene antidot lattices: Flat bands and spatial localization. Phys. Rev. B 80, 045410 (2009).
Eroms, J. & Weiss, D. Weak localization and transport gap in graphene antidot lattices. New J. Phys. 11, 095021 (2009).
Sofo, J. O., Chaudhari, A. S. & Barber, G. D. Graphane: A two-dimensional hydrocarbon. Phys. Rev. B 75, 153401 (2007).
Zhou, J., Wu, M. M., Zhou, X. & Sun, Q. Tuning electronic and magnetic properties of graphene by surface modification. Appl. Phys. Lett. 95, 103108 (2009).
Bostwick, A. et al. Quasiparticle transformation during a metal–insulator transition in graphene. Phys. Rev. Lett. 103, 1–4 (2009).
Elias, D. et al. Control of graphene’s properties by reversible hydrogenation: Evidence for graphane. Science 323, 610–613 (2009).
Guisinger, N., Rutter, G., Crain, J., First, P. & Stroscio, J. Exposure of epitaxial graphene on SiC(0001) to atomic hydrogen. Nano Lett. 9, 1462–1466 (2009).
Balog, R. et al. Atomic hydrogen adsorbate structures on graphene. J. Am. Chem. Soc. 131, 8744–8745 (2009).
Pletikosic, I. et al. Dirac cones and minigaps for graphene on Ir(111). Phys. Rev. Lett. 102, 056808 (2009).
Coraux, J., N′Diaye, A. T., Busse, C. & Michely, T. Structural coherency of graphene on Ir(111). Nano Lett. 8, 565–570 (2008).
N′Diaye, A. T., Bleikamp, S., Feibelman, P. J. & Michely, T. Two-dimensional Ir cluster lattice on a graphene moire on Ir(111). Phys. Rev. Lett. 97, 215501 (2006).
Feibelman, P. J. Pinning of graphene to Ir(111) by flat Ir dots. Phys. Rev. B 77, 165419 (2008).
Hornekaer, L. et al. Metastable structures and recombination pathways for atomic hydrogen on the graphite (0001) surface. Phys. Rev. Lett. 96, 156104 (2006).
Casolo, S., Lovvik, O. M., Martinazzo, R. & Tantardini, G. F. Understanding adsorption of hydrogen atoms on graphene. J. Chem. Phys. 130, 054704 (2009).
Boukhvalov, D. W. Hydrogen on graphene: Electronic structure, total energy, structural distortions and magnetism from first-principles calculations. Phys. Rev. B 77, 035427 (2008).
Ferro, Y. et al. Stability and magnetism of hydrogen dimers on graphene. Phys. Rev. B 78, 085417 (2008).
Acknowledgements
The authors gratefully acknowledge financial support from the European Research Council under ERC starting grant HPAH, no. 208344, The Danish Council for Independent Research and the Lundbeck Foundation. M.B. thanks the University of Trieste and Aarhus University (AU) for supporting his stay at AU. The research leading to these results has received financial support from the European Community’s Seventh Framework Programme (FP7/2007-2013) under grant agreement no. 226716.
Author information
Authors and Affiliations
Contributions
P.H. and L.H. planned the project; R.B., B.J., L.N., S.L., P.H. and L.H. designed the experiments; A.B. and S.L. supplied the procedure for graphene preparation; R.B., B.J., E.R., M.B., M.F., S.L. and P.H. carried out the UPS measurements; R.B., L.N. and M.A. carried out the STM measurements; E.L. provided technical support for the STM measurements; Z.S. and T.G.P. carried out the calculations; R.B., B.J., L.N., M.A., E.R., S.L., B.H., T.G.P., P.H. and L.H. analysed the data and interpreted the results; R.B., P.H. and L.H. wrote the manuscript; A.B., E.L., F.B. and B.H. advised on the project; all authors discussed the results and commented on the manuscript.
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing financial interests.
Supplementary information
Supplementary Information
Supplementary Information (PDF 3481 kb)
Rights and permissions
About this article
Cite this article
Balog, R., Jørgensen, B., Nilsson, L. et al. Bandgap opening in graphene induced by patterned hydrogen adsorption. Nature Mater 9, 315–319 (2010). https://doi.org/10.1038/nmat2710
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/nmat2710
This article is cited by
-
Exploring the adsorption performance of doped graphene quantum dots as anticancer drug carriers for cisplatin by DFT, PCM, and COSMO approaches
Structural Chemistry (2023)
-
Two-dimensional Stiefel-Whitney insulators in liganded Xenes
npj Computational Materials (2022)
-
Structure search of two-dimensional systems using CALYPSO methodology
Frontiers of Physics (2022)
-
Enhanced Removal of Diesel Oil Using New Magnetic Bentonite-Based Adsorbents Combined with Different Carbon Sources
Water, Air, & Soil Pollution (2022)
-
Unraveling the phonon scattering mechanism in exfoliated MoSe2 nanosheets using temperature-dependent Raman spectroscopy
Journal of Materials Science: Materials in Electronics (2022)