The structural modification and magnetism of many-layer epitaxial graphene implanted with low-energy light ions

Mazza, Alessandro R.; Miettinen, Anna; Gai, Zheng; He, Xiaoqing; Charlton, Timothy R.; Ward, Thomas Z.; Conrad, Matthew; Bian, Guang; Conrad, Edward H.; Miceli, Paul F.

doi:10.1016/j.carbon.2022.02.046

Title: The structural modification and magnetism of many-layer epitaxial graphene implanted with low-energy light ions

Journal Article · 24 February 2022 · Carbon

DOI: https://doi.org/10.1016/j.carbon.2022.02.046 · OSTI ID:1855644

^[1];

^[2];

^[3]; He, Xiaoqing ^[4];

^[3];

^[3]; Conrad, Matthew ^[2]; Bian, Guang ^[4];

^[2];

^[4]

Univ. of Missouri, Columbia, MO (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Georgia Inst. of Technology, Atlanta, GA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Missouri, Columbia, MO (United States)

Modifying the properties of graphene has gained wide interest for a plethora of potential applications, including spintronics. One approach has demonstrated that proton irradiation can induce ferromagnetism in graphene as well as in graphite. However, little is known about how the protons interact with graphene, the mechanism that creates the ferromagnetism, or whether the protons remain in the graphene. Here we report an investigation, broadly relevant to graphitic carbon, using low-energy (360–2000 eV) ions of hydrogen, deuterium, and helium implanted into multilayer epitaxial graphene. Complementary x-ray and neutron reflectivity demonstrate that essentially all of the implanted hydrogen remains chemisorbed in graphene. In situ x-ray diffraction reveals significantly different rates of interlayer expansion of the multilayer graphene. Analysis of these data demonstrates that the interlayer expansion arises entirely from the interstitials created by the ions and not from hydrogen that remains in the graphene. The results also establish a quantitative measure of the layer expansion due to carbon interstitials. Magnetometry and x-ray diffraction studies show that the magnetic moment relates to the amount of interstitial carbon rather than the amount of hydrogen, demonstrating that the induced room-temperature ferromagnetism arises directly from the disrupted bonding of the carbon lattice.

View Accepted Manuscript (DOE)

Cite

Export

Save

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; SC0014664

OSTI ID:: 1855644

Journal Information:: Carbon, Journal Name: Carbon Journal Issue: 1 Vol. 192; ISSN 0008-6223

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (56)

Field-Induced Transition from Room-Temperature Ferromagnetism to Diamagnetism in Proton-Irradiated Fullerene Lee, Kyu Won; Kweon, Hyocheon; Lee, Cheol Eui Advanced Materials, Vol. 25, Issue 39 https://doi.org/10.1002/adma201301635	journal	August 2013
Hydrogenated Graphenes by Birch Reduction: Influence of Electron and Proton Sources on Hydrogenation Efficiency, Magnetism, and Electrochemistry Eng, Alex Yong Sheng; Sofer, Zdeněk; Huber, Štěpán Chemistry - A European Journal, Vol. 21, Issue 47 https://doi.org/10.1002/chem.201503219	journal	October 2015
Recent Advances in Nanomaterial-Modified Pencil Graphite Electrodes for Electroanalysis Akanda, Md. Rajibul; Sohail, Manzar; Aziz, Md. Abdul Electroanalysis, Vol. 28, Issue 3 https://doi.org/10.1002/elan.201500374	journal	August 2015
Magnetism in graphite induced by irradiation of hydrogen or helium ions - A comparative study Makarova, Tatiana L.; Shelankov, Andrei L.; Serenkov, Igor T. physica status solidi (b), Vol. 247, Issue 11-12 https://doi.org/10.1002/pssb.201000114	journal	August 2010
Nuclear graphite—The first years Eatherly, W. P. Journal of Nuclear Materials, Vol. 100, Issue 1-3 https://doi.org/10.1016/0022-3115(81)90519-5	journal	September 1981
High resolution electron microscopy of graphite defect structures after KeV hydrogen ion bombardment Gotoh, Yoshitaka; Shimizu, Hazime; Murakami, Hiroshi Journal of Nuclear Materials, Vol. 162-164 https://doi.org/10.1016/0022-3115(89)90373-5	journal	April 1989
High resolution electron microscopy of graphite defect structures after keV hydrogen ion bombardment at elevated temperatures Hazime, Shimizu; Shigemi, Suginuma; Yoshitaka, Gotoh Journal of Nuclear Materials, Vol. 176-177 https://doi.org/10.1016/0022-3115(90)90181-L	journal	December 1990
A model of hydrogen implantation into graphite including bulk recombination by tunneling Brice, D. K. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 52, Issue 2 https://doi.org/10.1016/0168-583X(90)90582-F	journal	December 1990
Interlayer structure changes of graphite after hydrogen ion irradiation Gotoh, Yoshitaka Journal of Nuclear Materials, Vol. 248 https://doi.org/10.1016/S0022-3115(97)00115-3	journal	September 1997
Proton beam writing Watt, Frank; Breese, Mark B. H.; Bettiol, Andrew A. Materials Today, Vol. 10, Issue 6 https://doi.org/10.1016/S1369-7021(07)70129-3	journal	June 2007
Enhancing the ferromagnetization of graphite by successive 12C+ ion implantation steps He, Zhoutong; Yang, Xinmei; Xia, Huihao Carbon, Vol. 49, Issue 6 https://doi.org/10.1016/j.carbon.2011.01.018	journal	May 2011
Spatial variability in the mechanical properties of Gilsocarbon Arregui-Mena, José David; Bodel, William; Worth, Robert N. Carbon, Vol. 110 https://doi.org/10.1016/j.carbon.2016.09.051	journal	December 2016
Effect of boron and nitrogen doping with native point defects on the vibrational properties of graphene Islam, Md. Sherajul; Ushida, Kenji; Tanaka, Satoru Computational Materials Science, Vol. 94 https://doi.org/10.1016/j.commatsci.2014.01.040	journal	November 2014
3D-Hydrogen analysis of ferromagnetic microstructures in proton irradiated graphite Reichart, P.; Spemann, D.; Hauptner, A. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 249, Issue 1-2 https://doi.org/10.1016/j.nimb.2006.04.014	journal	August 2006
SRIM – The stopping and range of ions in matter (2010) Ziegler, James F.; Ziegler, M. D.; Biersack, J. P. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 268, Issue 11-12 https://doi.org/10.1016/j.nimb.2010.02.091	journal	June 2010
Modification on graphite due to helium ion irradiation Dutta, N. J.; Mohanty, S. R.; Buzarbaruah, N. Physics Letters A, Vol. 380, Issue 33 https://doi.org/10.1016/j.physleta.2016.05.044	journal	July 2016
Doping of Graphene by Low-Energy Ion Beam Implantation: Structural, Electronic, and Transport Properties Willke, Philip; Amani, Julian A.; Sinterhauf, Anna Nano Letters, Vol. 15, Issue 8 https://doi.org/10.1021/acs.nanolett.5b01280	journal	July 2015
Supraparamagnetic, Conductive, and Processable Multifunctional Graphene Nanosheets Coated with High-Density Fe ₃ O ₄ Nanoparticles He, Hongkun; Gao, Chao ACS Applied Materials & Interfaces, Vol. 2, Issue 11 https://doi.org/10.1021/am100673g	journal	October 2010
Graphene Oxide: Preparation, Functionalization, and Electrochemical Applications Chen, Da; Feng, Hongbin; Li, Jinghong Chemical Reviews, Vol. 112, Issue 11 https://doi.org/10.1021/cr300115g	journal	August 2012
Honeycomb Carbon: A Review of Graphene Allen, Matthew J.; Tung, Vincent C.; Kaner, Richard B. Chemical Reviews, Vol. 110, Issue 1, p. 132-145 https://doi.org/10.1021/cr900070d	journal	January 2010
Atomic Hydrogen Adsorbate Structures on Graphene Balog, Richard; Jørgensen, Bjarke; Wells, Justin Journal of the American Chemical Society, Vol. 131, Issue 25 https://doi.org/10.1021/ja902714h	journal	July 2009
Ion Implantation of Graphene—Toward IC Compatible Technologies Bangert, U.; Pierce, W.; Kepaptsoglou, D. M. Nano Letters, Vol. 13, Issue 10 https://doi.org/10.1021/nl402812y	journal	September 2013
Structural Defects in Graphene Banhart, Florian; Kotakoski, Jani; Krasheninnikov, Arkady V. ACS Nano, Vol. 5, Issue 1 https://doi.org/10.1021/nn102598m	journal	November 2010
Thickness-Dependent Reversible Hydrogenation of Graphene Layers Luo, Zhiqiang; Yu, Ting; Kim, Ki-jeong ACS Nano, Vol. 3, Issue 7 https://doi.org/10.1021/nn900371t	journal	June 2009
The rise of graphene Geim, A. K.; Novoselov, K. S. Nature Materials, Vol. 6, Issue 3, p. 183-191 https://doi.org/10.1038/nmat1849	journal	March 2007
Disorder in van der Waals heterostructures of 2D materials Rhodes, Daniel; Chae, Sang Hoon; Ribeiro-Palau, Rebeca Nature Materials, Vol. 18, Issue 6 https://doi.org/10.1038/s41563-019-0366-8	journal	May 2019
Van der Waals heterostructures for spintronics and opto-spintronics Sierra, Juan F.; Fabian, Jaroslav; Kawakami, Roland K. Nature Nanotechnology, Vol. 16, Issue 8 https://doi.org/10.1038/s41565-021-00936-x	journal	July 2021
Activation of radical addition to graphene by chemical hydrogenation Whitener, Keith E.; Lee, Woo-Kyung; Stine, Rory RSC Advances, Vol. 6, Issue 96 https://doi.org/10.1039/C6RA21113E	journal	January 2016
High-efficiency modulation of coupling between different polaritons in an in-plane graphene/hexagonal boron nitride heterostructure Guo, Xiangdong; Hu, Hai; Hu, Debo Nanoscale, Vol. 11, Issue 6 https://doi.org/10.1039/C8NR08334G	journal	January 2019
Revealing interfacial disorder at the growth-front of thick many-layer epitaxial graphene on SiC: a complementary neutron and X-ray scattering investigation Mazza, A. R.; Miettinen, A.; Daykin, A. A. Nanoscale, Vol. 11, Issue 30 https://doi.org/10.1039/C9NR03504D	journal	January 2019
Proton irradiation of graphene: insights from atomistic modeling Shi, Tan; Peng, Qing; Bai, Zhitong Nanoscale, Vol. 11, Issue 43 https://doi.org/10.1039/C9NR06502D	journal	January 2019
The success story of graphite as a lithium-ion anode material – fundamentals, remaining challenges, and recent developments including silicon (oxide) composites Asenbauer, Jakob; Eisenmann, Tobias; Kuenzel, Matthias Sustainable Energy & Fuels, Vol. 4, Issue 11 https://doi.org/10.1039/D0SE00175A	journal	January 2020
Graphane and hydrogenated graphene Pumera, Martin; Wong, Colin Hong An Chemical Society Reviews, Vol. 42, Issue 14 https://doi.org/10.1039/c3cs60132c	journal	January 2013
Modeling of hydrogen implantation into graphite Möller, W.; Scherzer, B. M. U. Journal of Applied Physics, Vol. 64, Issue 10 https://doi.org/10.1063/1.341234	journal	November 1988
Modulating the electronic structures of graphene by controllable hydrogenation Luo, Zhiqiang; Shang, Jingzhi; Lim, Sanhua Applied Physics Letters, Vol. 97, Issue 23 https://doi.org/10.1063/1.3524217	journal	December 2010
Magnetism in MoS ₂ induced by proton irradiation Mathew, S.; Gopinadhan, K.; Chan, T. K. Applied Physics Letters, Vol. 101, Issue 10 https://doi.org/10.1063/1.4750237	journal	September 2012
Voltage contrast X-ray photoelectron spectroscopy reveals graphene-substrate interaction in graphene devices fabricated on the C- and Si- faces of SiC Aydogan, Pinar; Arslan, Engin; Cakmakyapan, Semih Applied Physics Letters, Vol. 107, Issue 12 https://doi.org/10.1063/1.4931725	journal	September 2015
Two-dimensional van der Waals materials Ajayan, Pulickel; Kim, Philip; Banerjee, Kaustav Physics Today, Vol. 69, Issue 9 https://doi.org/10.1063/PT.3.3297	journal	September 2016
Large area and structured epitaxial graphene produced by confinement controlled sublimation of silicon carbide de Heer, W. A.; Berger, C.; Ruan, M. Proceedings of the National Academy of Sciences, Vol. 108, Issue 41 https://doi.org/10.1073/pnas.1105113108	journal	September 2011
Advances in the chemical modification of epitaxial graphene Bekyarova, E.; Sarkar, S.; Niyogi, S. Journal of Physics D: Applied Physics, Vol. 45, Issue 15 https://doi.org/10.1088/0022-3727/45/15/154009	journal	March 2012
The role of hydrogen in room-temperature ferromagnetism at graphite surfaces Ohldag, H.; Esquinazi, P.; Arenholz, E. New Journal of Physics, Vol. 12, Issue 12 https://doi.org/10.1088/1367-2630/12/12/123012	journal	December 2010
Electronic structure of the substitutional vacancy in graphene: density-functional and Green's function studies Nanda, B. R. K.; Sherafati, M.; Popović, Z. S. New Journal of Physics, Vol. 14, Issue 8 https://doi.org/10.1088/1367-2630/14/8/083004	journal	August 2012
Effect of helium implantation on SiC and graphite Guo, Hong-Yan; Ge, Chang-Chun; Xia, Min Chinese Physics B, Vol. 24, Issue 3 https://doi.org/10.1088/1674-1056/24/3/037803	journal	February 2015
Structural characterization of ion-implanted graphite Elman, B. S.; Shayegan, M.; Dresselhaus, M. S. Physical Review B, Vol. 25, Issue 6 https://doi.org/10.1103/PhysRevB.25.4142	journal	March 1982
Ferromagnetism in oriented graphite samples Esquinazi, P.; Setzer, A.; Höhne, R. Physical Review B, Vol. 66, Issue 2 https://doi.org/10.1103/PhysRevB.66.024429	journal	July 2002
Defect-induced magnetism in graphene Yazyev, Oleg V.; Helm, Lothar Physical Review B, Vol. 75, Issue 12 https://doi.org/10.1103/PhysRevB.75.125408	journal	March 2007
Anisotropic magnetism of graphite irradiated with medium-energy hydrogen and helium ions Makarova, T. L.; Shelankov, A. L.; Serenkov, I. T. Physical Review B, Vol. 83, Issue 8 https://doi.org/10.1103/PhysRevB.83.085417	journal	February 2011
Ab initio studies of hydrogen adatoms on bilayer graphene Mapasha, R. E.; Ukpong, A. M.; Chetty, N. Physical Review B, Vol. 85, Issue 20 https://doi.org/10.1103/PhysRevB.85.205402	journal	May 2012
Missing Atom as a Source of Carbon Magnetism Ugeda, M. M.; Brihuega, I.; Guinea, F. Physical Review Letters, Vol. 104, Issue 9 https://doi.org/10.1103/PhysRevLett.104.096804	journal	March 2010
Two theorems on the Hubbard model Lieb, Elliott H. Physical Review Letters, Vol. 62, Issue 10 https://doi.org/10.1103/PhysRevLett.62.1201	journal	March 1989
Induced Magnetic Ordering by Proton Irradiation in Graphite Esquinazi, P.; Spemann, D.; Höhne, R. Physical Review Letters, Vol. 91, Issue 22 https://doi.org/10.1103/PhysRevLett.91.227201	journal	November 2003
Electron Spin Resonance of Proton-Irradiated Graphite Lee, Kyu Won; Lee, Cheol Eui Physical Review Letters, Vol. 97, Issue 13 https://doi.org/10.1103/PhysRevLett.97.137206	journal	September 2006
π -Electron Ferromagnetism in Metal-Free Carbon Probed by Soft X-Ray Dichroism Ohldag, H.; Tyliszczak, T.; Höhne, R. Physical Review Letters, Vol. 98, Issue 18 https://doi.org/10.1103/PhysRevLett.98.187204	journal	May 2007
2D materials and van der Waals heterostructures Novoselov, K. S.; Mishchenko, A.; Carvalho, A. Science, Vol. 353, Issue 6298 https://doi.org/10.1126/science.aac9439	journal	July 2016
Atomic-scale control of graphene magnetism by using hydrogen atoms Gonzalez-Herrero, H.; Gomez-Rodriguez, J. M.; Mallet, P. Science, Vol. 352, Issue 6284 https://doi.org/10.1126/science.aad8038	journal	April 2016
Blast Furnace Hearth Lining: Post Mortem Analysis Almeida, Bruno Vidal de; Neves, Elton Silva; Silva, Sidiney Nascimento Materials Research, Vol. 20, Issue 3 https://doi.org/10.1590/1980-5373-mr-2016-0875	journal	May 2017

Similar Records

Disorder and hydrogenation in graphene nanopowder revealed by complementary X-ray and neutron scattering

Journal Article · 2023 · Carbon · OSTI ID:1924423

Daykin, Alexander A.; Ravula, Sudhir; Kaiser, Helmut; +6 more

Atomic deuteration of epitaxial many-layer graphene on 4H-SiC(000$\bar{1}$)

Journal Article · 2019 · Journal of Vacuum Science and Technology B · OSTI ID:1558512

Mazza, Alessandro R.; Miettinen, Anna; Conrad, Matt; +7 more

Synthesis of Room-Temperature Ferromagnetic Cr-doped TiO₂(110) Rutile Single Crystals using Ion Implantation

Journal Article · 2005 · Nuclear Instruments and Methods in Physics Research. Section B, Beam Interactions with Materials and Atoms, 242(1-2):198-200 · OSTI ID:881927

Shutthanandan, V.; Thevuthasan, Suntharampillai; Droubay, Timothy C.; +6 more

Related Subjects

36 MATERIALS SCIENCE

Title: The structural modification and magnetism of many-layer epitaxial graphene implanted with low-energy light ions

Citation Formats

References (56)

Similar Records

Related Subjects