In Situ Observations of the Atomistic Mechanisms of Ni Catalyzed Low Temperature Graphene Growth
Patera, Laerte L
American Chemical Society
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Patera, L. L., Africh, C., Weatherup, R., Blume, R., Bhardwaj, S., Castellarin-Cudia, C., Knop-Gericke, A., et al. (2013). In Situ Observations of the Atomistic Mechanisms of Ni Catalyzed Low Temperature Graphene Growth. ACS Nano, 7901-7912. https://doi.org/10.1021/nn402927q
The key atomistic mechanisms of graphene formation on Ni for technologically relevant hydrocarbon exposures below 600°C are directly revealed via complementary in situ scanning tunneling microscopy and Xray photoelectron spectroscopy. For clean Ni(111) below 500°C, two different surface carbide (Ni2C) conversion mechanisms are dominant which both yield epitaxial graphene, whereas above 500°C graphene predominantly grows directly on Ni(111) via replacement mechanisms leading to embedded epitaxial and/or rotated graphene domains. Upon cooling, additional carbon structures form exclusively underneath rotated graphene domains. The dominant graphene growth mechanism also critically depends on the near-surface carbon concentration and hence is intimately linked to the full history of the catalyst and all possible sources of contamination. The detailed XPS fingerprinting of these processes allows a direct link to high pressure XPS measurements of a wide range of growth conditions, including polycrystalline Ni catalysts and recipes commonly used in industrial reactors for graphene and carbon nanotube CVD. This enables an unambiguous and consistent interpretation of prior literature and an assessment of how the quality/structure of as-grown carbon nanostructures relates to the growth modes.
Graphene, Chemical vapor deposition (CVD), Ni, surface carbide, Scanning Tunneling Microscopy (STM), X-ray photoelectron spectroscopy (XPS)
L.L.P. acknowledges funding from Area di Ricerca Scientifica e Tecnologica of Trieste and from MIUR through Progetto Strategico NFFA. C.A. acknowledges support from CNR through the ESF FANAS project NOMCIS. C.A. and C.C. acknowledge financial support from MIUR (PRIN 2010-2011 nº 2010N3T9M4). S.B. acknowledges funding from ICTP TRIL program. S.H. acknowledges funding from ERC grant InsituNANO (n°279342). R.S.W. acknowledges funding from EPSRC (Doctoral training award), and the Nano Science & Technology Doctoral Training Centre Cambridge (NanoDTC). The help of C. Dri and F. Esch (design) and P. Bertoch and F. Salvador (manufacturing) in the realization of the high temperature STM sample holder is gratefully acknowledged. We acknowledge the Helmholtz-Zentrum-Berlin Electron storage ring BESSY II for provision of synchrotron radiation at the ISISS beamline and we thank the BESSY staff for continuous support of our experiments.
European Research Council (279342)
External DOI: https://doi.org/10.1021/nn402927q
This record's URL: https://www.repository.cam.ac.uk/handle/1810/246854