Abstract
Controlling the atomic configurations of structural defects in graphene nanostructures is crucial for achieving desired functionalities. Here, we report the controlled fabrication of high-quality single-crystal and bicrystal graphene nanoislands (GNI) through a unique top-down etching and post-annealing procedure on a graphite surface. Low-temperature scanning tunneling microscopy (STM) combined with density functional theory calculations reveal that most of grain boundaries (GBs) formed on the bicrystal GNIs are 5-7-5-7 GBs. Two nanodomains separated by a 5-7-5-7 GB are AB stacking and twisted stacking with respect to the underlying graphite substrate and exhibit distinct electronic properties, forming a graphene homojunction. In addition, we construct homojunctions with alternative AB/twisted stacking nanodomains separated by parallel 5-7-5-7 GBs. Remarkably, the stacking orders of homojunctions are manipulated from AB/twist into twist/twist type through a STM tip. The controllable fabrication and manipulation of graphene homojunctions with 5-7-5-7 GBs and distinct stacking orders open an avenue for the construction of GBs-based devices in valleytronics and twistronics.
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Mishra, S.; Beyer, D.; Eimre, K.; Kezilebieke, S.; Berger, R.; Gröning, O.; Pignedoli, C. A.; Müllen, K.; Liljeroth, P. et al. Topological frustration induces unconventional magnetism in a nanographene. Nat. Nanotechnol. 2020, 15, 81.
Cox, J. D.; García de Abajo, F. J. Nonlinear interactions between free electrons and nanographenes. Nano Lett. 2020, 20, 4792–4800.
Cox, J. D.; de Abajo, F. J. G Single-plasmon thermo-optical switching in graphene. Nano Lett. 2019, 19, 3743–3750.
Su, J.; Telychko, M.; Hu, P.; Macam, G.; Mutombo, P.; Zhang, H. J.; Bao, Y.; Cheng, F.; Huang, Z. Q.; Qiu, Z. Z. et al. Atomically precise bottom-up synthesis of π-extended [5]triangulene. Sci. Adv. 2019, 5, eaav7717.
Chen, H.; Que, Y. D.; Tao, L.; Zhang, Y. Y.; Lin, X.; Xiao, W. D.; Wang, D. F.; Du, S. X.; Pantelides, S. T.; Gao, H. J. Recovery of edge states of graphene nanoislands on an iridium substrate by silicon intercalation. Nano Res. 2018, 11, 3722–3729.
Pavliček, N.; Mistry, A.; Majzik, Z.; Moll, N.; Meyer, G.; Fox, D. J.; Gross, L. Synthesis and characterization of triangulene. Nat. Nanotechnol. 2017, 12, 308–311.
Leicht, P.; Zielke, L.; Bouvron, S.; Moroni, R.; Voloshina, E.; Hammerschmidt, L.; Dedkov, Y. S.; Fonin, M. In situ fabrication of quasi-free-standing epitaxial graphene nanoflakes on gold. ACS Nano 2014, 8, 3735–3742.
Phark, S. H.; Borme, J.; Vanegas, A. L.; Corbetta, M.; Sander, D.; Kirschner, J. Direct observation of electron confinement in epitaxial graphene nanoislands. ACS Nano 2011, 5, 8162–8166.
Fernández-Rossier, J.; Palacios, J. J. Magnetism in graphene nanoislands. Phys. Rev. Lett. 2007, 99, 177204.
Feng, X. F.; Kwon, S.; Park, J. Y.; Salmeron, M. Superlubric sliding of graphene nanoflakes on graphene. ACS Nano 2013, 7, 1718–1724.
Zhu, S. Z.; Li, T. Hydrogenation-assisted graphene origami and its application in programmable molecular mass uptake, storage, and release. ACS Nano 2014, 8, 2864–2872.
Chen, H.; Zhang, X. L.; Zhang, Y. Y.; Wang, D. F.; Bao, D. L.; Que, Y. D.; Xiao, W. D.; Du, S. X.; Ouyang, M.; Pantelides, S. T. et al. Atomically precise, custom-design origami graphene nanostructures. Science 2019, 365, 1036–1040.
Wilson, P. M.; Mbah, G. N.; Smith, T. G.; Schmidt, D.; Lai, R. Y.; Hofmann, T.; Sinitskii, A. Three-dimensional periodic graphene nanostructures. J. Mater. Chem. C 2014, 2, 1879–1886.
Heerema, S. J.; Dekker, C. Graphene nanodevices for DNA sequencing. Nat. Nanotechnol. 2016, 11, 127–136.
Majee, A. K.; Kommini, A.; Aksamija, Z. Electronic transport and thermopower in 2D and 3D heterostructures—A theory perspective. Ann. Phys. 2019, 531, 1800510.
Yazyev, O. V.; Louie, S. G. Electronic transport in polycrystalline graphene. Nat. Mater. 2010, 9, 806–809.
Gunlycke, D.; White, C. T. Graphene valley filter using a line defect. Phys. Rev. Lett. 2011, 106, 136806.
Chen, J. H.; Autès, G.; Alem, N.; Gargiulo, F.; Gautam, A.; Linck, M.; Kisielowski, C.; Yazyev, O. V.; Louie, S. G.; Zettl, A. Controlled growth of a line defect in graphene and implications for gate-tunable valley filtering. Phys. Rev. B 2014, 89, 121407(R).
Xu, J.; Yuan, G. W.; Zhu, Q.; Wang, J. W.; Tang, S.; Gao, L. B. Enhancing the strength of graphene by a denser grain boundary. ACS Nano 2018, 12, 4529–4535.
Alexandre, S. S.; Lúcio, A. D.; Neto, A. H. C.; Nunes, R. W. Correlated magnetic states in extended one-dimensional defects in graphene. Nano Lett. 2012, 12, 5097–5102.
Kou, L. Z.; Tang, C.; Guo, W. L.; Chen, C. F. Tunable magnetism in strained graphene with topological line defect. ACS Nano 2011, 5, 1012–1017.
Wu, H. C.; Chaika, A. N.; Hsu, M. C.; Huang, T. W.; Abid, M.; Abid, M.; Aristov, V. Y.; Molodtsova, O. V.; Babenkov, S. V.; Niu, Y. R. et al. Large positive in-plane magnetoresistance induced by localized states at nanodomain boundaries in graphene. Nat. Commun. 2017, 8, 14453.
Gunlycke, D.; Vasudevan, S.; White, C. T. Confinement, transport gap, and valley polarization in graphene from two parallel decorated line defects. Nano Lett. 2013, 13, 259–263.
Biró, L. P.; Lambin, P. Grain boundaries in graphene grown by chemical vapor deposition. New J. Phys. 2013, 15, 035024.
Tison, Y.; Lagoute, J.; Repain, V.; Chacon, C.; Girard, Y.; Joucken, F.; Sporken, R.; Gargiulo, F.; Yazyev, O. V.; Rousset, S. Grain boundaries in graphene on SiC(0001) substrate. Nano Lett. 2014, 14, 6382–6386.
Yang, B.; Xu, H.; Lu, J.; Loh, K. P. Periodic grain boundaries formed by thermal reconstruction of polycrystalline graphene film. J. Am. Chem. Soc. 2014, 136, 12041–12046.
Chen, Y. B.; Sun, J. Y.; Gao, J. F.; Du, F.; Han, Q.; Nie, Y. F.; Chen, Z. L.; Bachmatiuk, A.; Priydarshi, M. K.; Ma, D. L. et al. Growing uniform graphene disks and films on molten glass for heating devices and cell culture. Adv. Mater. 2015, 27, 7839–7846.
Yazyev, O. V.; Louie, S. G Topological defects in graphene: Dislocations and grain boundaries. Phys. Rev. B 2010, 81, 195420.
Katsnelson, M. I.; Novoselov, K. S.; Geim, A. K. Chiral tunnelling and the klein paradox in graphene. Nat. Phys. 2006, 2, 620–625.
Cao, Y.; Fatemi, V.; Fang, S. A.; Watanabe, K.; Taniguchi, T.; Kaxiras, E.; Jarillo-Herrero, P. Unconventional superconductivity in magic-angle graphene superlattices. Nature 2018, 556, 43–50.
Cao, Y.; Fatemi, V.; Demir, A.; Fang, S. A.; Tomarken, S. L.; Luo, J. Y.; Sanchez-Yamagishi, J. D.; Watanabe, K.; Taniguchi, T.; Kaxiras, E. et al. Correlated insulator behaviour at half-filling in magic-angle graphene superlattices. Nature 2018, 556, 80–84.
Sharpe, A. L.; Fox, E. J.; Barnard, A. W.; Finney, J.; Watanabe, K.; Taniguchi, T.; Kastner, M. A.; Goldhaber-Gordon, D. Emergent ferromagnetism near three-quarters filling in twisted bilayer graphene. Science 2019, 365, 605–608.
Lin, J. H.; Fang, W. J.; Zhou, W.; Lupini, A. R.; Idrobo, J. C.; Kong, J.; Pennycook, S. J.; Pantelides, S. T. AC/AB stacking boundaries in bilayer graphene. Nano Lett. 2013, 13, 3262–3268.
Kim, C. J.; Sánchez-Castillo, A.; Ziegler, Z.; Ogawa, Y.; Noguez, C.; Park, J. Chiral atomically thin films. Nat. Nanotechnol. 2016, 11, 520–524.
Hikino, S.; Yunoki, S. Anomalous enhancement of spin Hall conductivity in a superconductor/normal-metal junction. Phys. Rev. B 2011, 84, 020512(R).
Yang, R.; Zhang, L. C.; Wang, Y.; Shi, Z. W.; Shi, D. X.; Gao, H. J.; Wang, E. G.; Zhang, G. Y. An anisotropic etching effect in the graphene basal plane. Adv. Mater. 2010, 22, 4014–4019.
Kresse, G.; Joubert, D. From ultrasoft pseudopotentials to the projector augmented-wave method. Phys. Rev. B 1999, 59, 1758–1775.
Vanderbilt, D. Soft self-consistent pseudopotentials in a generalized eigenvalue formalism. Phys. Rev. B 1990, 41, 7892–7895.
Kresse, G.; Furthmüller, J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys. Rev. B 1996, 54, 11169–11186.
Perdew, J. P.; Zunger, A. Self-interaction correction to density-functional approximations for many-electron systems. Phys. Rev. B 1981, 23, 5048–5079.
Acknowledgements
We thank Sokrates T. Pantelides and Min Ouyang for constructive suggestions. We acknowledge financial support from the National Key Research & Development Projects of China (Nos. 2016YFA0202300 and 2019YFA0308500), the National Natural Science Foundation of China (Nos. 61888102, 51872284, 51922011, 11974045, and 51761135130), the CAS Pioneer Hundred Talents Program, Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDB30000000), and China Postdoctoral Science Foundation (Nos. 2018M641511, 2018M630217, and 2019T120148). A portion of the research was performed in CAS Key Laboratory of Vacuum Physics.
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Chen, H., Bao, DL., Wang, D. et al. Fabrication and manipulation of nanosized graphene homojunction with atomically-controlled boundaries. Nano Res. 13, 3286–3291 (2020). https://doi.org/10.1007/s12274-020-3004-5
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DOI: https://doi.org/10.1007/s12274-020-3004-5