Energy barriers for Dy and H penetrating graphene on 6H-SiC(0001) and freestanding bilayer graphene from first-principles calculations

Han, Yong; Evans, James W.; Tringides, Michael C.

doi:10.1063/5.0056916

Energy barriers for Dy and H penetrating graphene on 6H-SiC(0001) and freestanding bilayer graphene from first-principles calculations

Journal Article · Tue Jul 20 00:00:00 EDT 2021 · Applied Physics Letters

DOI:https://doi.org/10.1063/5.0056916· OSTI ID:1817665

^[1]; ^[1]; ^[1]

Ames Lab., and Iowa State Univ., Ames, IA (United States)

Currently, intercalation of foreign guest atoms into two-dimensional (2D) layered van der Waals materials is an active research area motivated in part by the development of next-generation energy-storage technologies and optoelectronic devices. One such extensively studied 2D material is the graphene-on-SiC system. To realize and control the desired intercalated structures, it is fundamentally important to understand the kinetic process of intercalation. For the intercalation of a guest atom into graphene layers on SiC substrate, a critical kinetic parameter is the energy barrier of a guest atom penetrating the perfect graphene top layer into the gallery under it. However, accurate theoretical calculations for such penetration barriers are unavailable in literature. From our first-principles density functional theory calculations, we obtain the global energy barriers of 3.47 and 1.80 eV for single Dy and H atoms penetrating the graphene top layer on a graphene buffer layer supported by a Si-terminated 6H-SiC(0001) substrate, respectively. Furthermore, for comparison as well as for examining the lateral strain effects, we also obtain the global barriers of 5.05 and 1.50 eV for single Dy and H atoms penetrating freestanding bilayer graphene with a tensile strain of about 8.8% to match our model for supported graphene, as well as the global barriers of 7.21 and 4.18 eV for penetrating unstrained freestanding bilayer graphene, respectively. From corresponding minimum energy paths with multiple energy minima and saddle points, we can also obtain various local energy barriers and the global backward barrier from the graphene gallery back to the top surface.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-05CH11231; AC02-07CH11358

OSTI ID:: 1817665

Alternate ID(s):: OSTI ID: 1808728

Report Number(s):: IS--J 10,547

Journal Information:: Applied Physics Letters, Journal Name: Applied Physics Letters Journal Issue: 3 Vol. 119; ISSN 0003-6951

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

References (49)

Intercalation of Layered Materials from Bulk to 2D Stark, Madeline S.; Kuntz, Kaci L.; Martens, Sean J. Advanced Materials, Vol. 31, Issue 27 https://doi.org/10.1002/adma.201808213	journal	May 2019
Hydrogenation of the buffer-layer graphene on 6H-SiC (0001): A possible route for the engineering of graphene-based devices Lin, Yu-Pu; Ksari, Younal; Themlin, Jean-Marc Nano Research, Vol. 8, Issue 3 https://doi.org/10.1007/s12274-014-0566-0	journal	September 2014
Intercalation of H at the graphene/SiC(0001) interface: Structure and stability from first principles Sclauzero, Gabriele; Pasquarello, Alfredo Applied Surface Science, Vol. 291 https://doi.org/10.1016/j.apsusc.2013.09.031	journal	February 2014
Manipulation of Dirac cones in intercalated epitaxial graphene Kim, Minsung; Tringides, Michael C.; Hershberger, Matthew T. Carbon, Vol. 123 https://doi.org/10.1016/j.carbon.2017.07.020	journal	October 2017
Doping modulation of quasi-free-standing monolayer graphene formed on SiC(0001) through Sn1-Ge intercalation Kim, Hidong; Dugerjav, Otgonbayar; Lkhagvasuren, Altaibaatar Carbon, Vol. 144 https://doi.org/10.1016/j.carbon.2018.12.084	journal	April 2019
Intercalated rare-earth metals under graphene on SiC Anderson, Nathaniel A.; Hupalo, Myron; Keavney, David Journal of Magnetism and Magnetic Materials, Vol. 474 https://doi.org/10.1016/j.jmmm.2018.11.007	journal	March 2019
Functionalization of 2D materials by intercalation Daukiya, L.; Nair, M. N.; Cranney, M. Progress in Surface Science, Vol. 94, Issue 1 https://doi.org/10.1016/j.progsurf.2018.07.001	journal	February 2019
Buffer layer free large area bi-layer graphene on SiC(0001) Virojanadara, C.; Zakharov, A. A.; Yakimova, R. Surface Science, Vol. 604, Issue 2 https://doi.org/10.1016/j.susc.2009.11.011	journal	January 2010
Hydrogen intercalation of graphene grown on 6H-SiC(0001) Watcharinyanon, S.; Virojanadara, C.; Osiecki, J. R. Surface Science, Vol. 605, Issue 17-18 https://doi.org/10.1016/j.susc.2010.12.018	journal	September 2011
Surface energies, adhesion energies, and exfoliation energies relevant to copper-graphene and copper-graphite systems Han, Yong; Lai, King C.; Lii-Rosales, Ann Surface Science, Vol. 685 https://doi.org/10.1016/j.susc.2019.01.009	journal	July 2019
Metal-dielectric transition in Sn-intercalated graphene on SiC(0001) Niu, Y. R.; Zakharov, A. A.; Yakimova, R. Ultramicroscopy, Vol. 183 https://doi.org/10.1016/j.ultramic.2017.05.010	journal	December 2017
Thermodynamic Preference for Atom Adsorption on versus Intercalation into Multilayer Graphene Li, Wei; Huang, Li; Tringides, Michael C. The Journal of Physical Chemistry Letters, Vol. 11, Issue 22 https://doi.org/10.1021/acs.jpclett.0c02887	journal	November 2020
Metal Adsorption and Nucleation on Free-Standing Graphene by Low-Energy Electron Point Source Microscopy Lorenzo, Marianna; Escher, Conrad; Latychevskaia, Tatiana Nano Letters, Vol. 18, Issue 6 https://doi.org/10.1021/acs.nanolett.8b00359	journal	May 2018
Superconducting Calcium-Intercalated Bilayer Graphene Ichinokura, Satoru; Sugawara, Katsuaki; Takayama, Akari ACS Nano, Vol. 10, Issue 2 https://doi.org/10.1021/acsnano.5b07848	journal	January 2016
Epitaxial Graphene Transistors: Enhancing Performance via Hydrogen Intercalation Robinson, Joshua A.; Hollander, Matthew; LaBella, Michael Nano Letters, Vol. 11, Issue 9 https://doi.org/10.1021/nl2019855	journal	September 2011
Quasi-Free-Standing Epitaxial Graphene on SiC (0001) by Fluorine Intercalation from a Molecular Source Wong, Swee Liang; Huang, Han; Wang, Yuzhan ACS Nano, Vol. 5, Issue 9 https://doi.org/10.1021/nn202910t	journal	August 2011
Classification of chemical bonds based on topological analysis of electron localization functions Silvi, B.; Savin, A. Nature, Vol. 371, Issue 6499 https://doi.org/10.1038/371683a0	journal	October 1994
Semiconductor to metal transition in two-dimensional gold and its van der Waals heterostack with graphene Forti, Stiven; Link, Stefan; Stöhr, Alexander Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-15683-1	journal	May 2020
Nuclear quantum effects enter the mainstream Markland, Thomas E.; Ceriotti, Michele Nature Reviews Chemistry, Vol. 2, Issue 3 https://doi.org/10.1038/s41570-017-0109	journal	February 2018
Spin-induced band modifications of graphene through intercalation of magnetic iron atoms Sung, S. J.; Yang, J. W.; Lee, P. R. Nanoscale, Vol. 6, Issue 7 https://doi.org/10.1039/C3NR04178F	journal	January 2014
Tuning two-dimensional nanomaterials by intercalation: materials, properties and applications Wan, Jiayu; Lacey, Steven D.; Dai, Jiaqi Chemical Society Reviews, Vol. 45, Issue 24 https://doi.org/10.1039/C5CS00758E	journal	January 2016
Epitaxial graphene/silicon carbide intercalation: a minireview on graphene modulation and unique 2D materials Briggs, Natalie; Gebeyehu, Zewdu M.; Vera, Alexander Nanoscale, Vol. 11, Issue 33 https://doi.org/10.1039/C9NR03721G	journal	January 2019
Penetration of alkali atoms throughout a graphene membrane: theoretical modeling Boukhvalov, D. W.; Virojanadara, C. Nanoscale, Vol. 4, Issue 5 https://doi.org/10.1039/c2nr11892k	journal	January 2012
Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points Henkelman, Graeme; Jónsson, Hannes The Journal of Chemical Physics, Vol. 113, Issue 22 https://doi.org/10.1063/1.1323224	journal	December 2000
The quasi-free-standing nature of graphene on H-saturated SiC(0001) Speck, F.; Jobst, J.; Fromm, F. Applied Physics Letters, Vol. 99, Issue 12 https://doi.org/10.1063/1.3643034	journal	September 2011
Superconductivity in Ca-intercalated epitaxial graphene on silicon carbide Li, Kang; Feng, Xiao; Zhang, Wenhao Applied Physics Letters, Vol. 103, Issue 6 https://doi.org/10.1063/1.4817781	journal	August 2013
Structural consequences of hydrogen intercalation of epitaxial graphene on SiC(0001) Emery, Jonathan D.; Wheeler, Virginia D.; Johns, James E. Applied Physics Letters, Vol. 105, Issue 16 https://doi.org/10.1063/1.4899142	journal	October 2014
Hydrogen intercalation of epitaxial graphene and buffer layer probed by mid-infrared absorption and Raman spectroscopy Kunc, J.; Rejhon, M.; Hlídek, P. AIP Advances, Vol. 8, Issue 4 https://doi.org/10.1063/1.5024132	journal	April 2018
Ca intercalated bilayer graphene as a thinnest limit of superconducting C6Ca Kanetani, K.; Sugawara, K.; Sato, T. Proceedings of the National Academy of Sciences, Vol. 109, Issue 48 https://doi.org/10.1073/pnas.1208889109	journal	November 2012
Evidence for superconductivity in Li-decorated monolayer graphene Ludbrook, B. M.; Levy, G.; Nigge, P. Proceedings of the National Academy of Sciences, Vol. 112, Issue 38 https://doi.org/10.1073/pnas.1510435112	journal	September 2015
Mini-Dirac cones in the band structure of a copper intercalated epitaxial graphene superlattice Forti, S.; Stöhr, A.; Zakharov, A. A. 2D Materials, Vol. 3, Issue 3 https://doi.org/10.1088/2053-1583/3/3/035003	journal	July 2016
Anisotropic Diffusion of a Charged Tritium Interstitial in Li 2 Ti O 3 from First-Principles Calculations Shi, Yanli; Qi, Jianqi; Han, Yong Physical Review Applied, Vol. 10, Issue 2 https://doi.org/10.1103/PhysRevApplied.10.024021	journal	August 2018
Unraveling anomalous isotope effect on hydrogen diffusivities in fcc metals from first principles including nuclear quantum effects Kimizuka, Hajime; Ogata, Shigenobu; Shiga, Motoyuki Physical Review B, Vol. 100, Issue 2 https://doi.org/10.1103/PhysRevB.100.024104	journal	July 2019
Tuning the doping level of graphene in the vicinity of the Van Hove singularity via ytterbium intercalation Rosenzweig, Philipp; Karakachian, Hrag; Link, Stefan Physical Review B, Vol. 100, Issue 3 https://doi.org/10.1103/PhysRevB.100.035445	journal	July 2019
Heteroepitaxial graphite on 6 H − SiC ( 0001 ) : Interface formation through conduction-band electronic structure Forbeaux, I.; Themlin, J. -M.; Debever, J. -M. Physical Review B, Vol. 58, Issue 24 https://doi.org/10.1103/PhysRevB.58.16396	journal	December 1998
Electronic decoupling of an epitaxial graphene monolayer by gold intercalation Gierz, Isabella; Suzuki, Takayuki; Weitz, R. Thomas Physical Review B, Vol. 81, Issue 23 https://doi.org/10.1103/PhysRevB.81.235408	journal	June 2010
Decoupling graphene from SiC(0001) via oxidation Oida, S.; McFeely, F. R.; Hannon, J. B. Physical Review B, Vol. 82, Issue 4 https://doi.org/10.1103/PhysRevB.82.041411	journal	July 2010
First-principles study of hydrogen and fluorine intercalation into graphene-SiC(0001) interface Markevich, A.; Jones, R.; Öberg, S. Physical Review B, Vol. 86, Issue 4 https://doi.org/10.1103/PhysRevB.86.045453	journal	July 2012
Electronic and geometric structure of graphene/SiC(0001) decoupled by lithium intercalation Bisti, F.; Profeta, G.; Vita, H. Physical Review B, Vol. 91, Issue 24 https://doi.org/10.1103/PhysRevB.91.245411	journal	June 2015
Charge neutrality in epitaxial graphene on 6 H -SiC(0001) via nitrogen intercalation Caffrey, Nuala M.; Armiento, Rickard; Yakimova, Rositsa Physical Review B, Vol. 92, Issue 8 https://doi.org/10.1103/PhysRevB.92.081409	journal	August 2015
Quasi-Free-Standing Epitaxial Graphene on SiC Obtained by Hydrogen Intercalation Riedl, C.; Coletti, C.; Iwasaki, T. Physical Review Letters, Vol. 103, Issue 24 https://doi.org/10.1103/PhysRevLett.103.246804	journal	December 2009
Extended van Hove Singularity and Superconducting Instability in Doped Graphene McChesney, J. L.; Bostwick, Aaron; Ohta, Taisuke Physical Review Letters, Vol. 104, Issue 13 https://doi.org/10.1103/PhysRevLett.104.136803	journal	April 2010
Approaching Truly Freestanding Graphene: The Structure of Hydrogen-Intercalated Graphene on 6 H − SiC ( 0001 ) Sforzini, J.; Nemec, L.; Denig, T. Physical Review Letters, Vol. 114, Issue 10 https://doi.org/10.1103/PhysRevLett.114.106804	journal	March 2015
Charge-Density Wave in Ca-Intercalated Bilayer Graphene Induced by Commensurate Lattice Matching Shimizu, Ryota; Sugawara, Katsuaki; Kanetani, Kohei Physical Review Letters, Vol. 114, Issue 14 https://doi.org/10.1103/PhysRevLett.114.146103	journal	April 2015
Ab Initio Study of Graphene on SiC Mattausch, Alexander; Pankratov, Oleg Physical Review Letters, Vol. 99, Issue 7 https://doi.org/10.1103/PhysRevLett.99.076802	journal	August 2007
Intrinsic stacking domains in graphene on silicon carbide: A pathway for intercalation de Jong, T. A.; Krasovskii, E. E.; Ott, C. Physical Review Materials, Vol. 2, Issue 10 https://doi.org/10.1103/PhysRevMaterials.2.104005	journal	October 2018
Dy adsorption on and intercalation under graphene on 6 H -SiC(0001) surface from first-principles calculations Han, Yong; Evans, James W.; Tringides, Michael C. Physical Review Materials, Vol. 5, Issue 7 https://doi.org/10.1103/PhysRevMaterials.5.074004	journal	July 2021
Controlling the Electronic Structure of Bilayer Graphene Ohta, Taisuke; Bostwick, Aaron; Seyller, Thomas Science, Vol. 313, Issue 5789 https://doi.org/10.1126/science.1130681	journal	August 2006
Quantum Hall Effect and Carrier Scattering in Quasi-Free-Standing Monolayer Graphene Tanabe, Shinichi; Takamura, Makoto; Harada, Yuichi Applied Physics Express, Vol. 5, Issue 12 https://doi.org/10.1143/APEX.5.125101	journal	November 2012

Similar Records

Dy adsorption on and intercalation under graphene on 6H-SiC(0001) surface from first-principles calculations

Journal Article · Tue Jul 20 20:00:00 EDT 2021 · Physical Review Materials · OSTI ID:1817655

Thermodynamics and kinetics of H adsorption and intercalation for graphene on 6H-SiC(0001) from first-principles calculations

Journal Article · Mon Dec 06 19:00:00 EST 2021 · Journal of Vacuum Science and Technology A · OSTI ID:1835555

Related Subjects

2D materials
71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
annealing
chemical bonding
crystallographic defects
density functional theory
energy storage
first-principle calculations
graphene
optoelectronic devices

Energy barriers for Dy and H penetrating graphene on 6H-SiC(0001) and freestanding bilayer graphene from first-principles calculations

Citation Formats

References (49)

Similar Records

Related Subjects