Atmospheric pressure graphitization of SiC(0001) – A route towards wafer-size graphene layers

Atmospheric pressure graphitization of SiC(0001) – A route towards wafer-size graphene layers

| Konstantin V. Emtsev¹, Aaron Bostwick², Karsten Horn³, Johannes Jobst⁴, Gary L. Kellogg⁵, Lothar Ley¹, Jessica L. McChesney², Taisuke Ohta⁵, Sergey A. Reshanov⁴, Eli Rotenberg², Andreas K. Schmid⁶, Daniel Waldmann⁴, Heiko B. Weber⁴, Thomas Seyller¹,*
This study presents a method for producing high-quality, large-scale graphene layers on SiC(0001) substrates through atmospheric pressure graphitization. The process involves ex-situ graphitization of Si-terminated SiC(0001) in an argon atmosphere at about 1 bar, resulting in monolayer graphene films with significantly larger domain sizes compared to previously achievable methods. Hall measurements confirm the quality of the films, with high electronic mobilities reaching 2000 cm²/Vs at 27 K. The mobility decreases linearly with increasing temperature, likely due to electron-electron interactions. The method offers a viable route for the synthesis of uniform, wafer-size graphene layers for technological applications. However, the large-scale structural quality is currently limited by the lack of continuity and uniformity of the grown film. The study compares the results of vacuum annealing with those of ex-situ annealing under argon atmosphere, showing that the latter produces significantly improved surface morphology. The surface undergoes considerable morphological changes during graphitization, leading to a more uniform and smoother surface. The improved surface morphology is attributed to the significantly higher annealing temperature (1650°C) required for graphene formation under argon at 900 mbar compared to 1280°C in UHV. The higher temperature enhances surface diffusion, allowing the restructuring of the surface before graphene formation, leading to a more uniform and smoother surface. The study also demonstrates that the graphene layers grown under argon atmosphere exhibit high structural and electronic quality, as evidenced by LEED and photoelectron spectroscopy data. The C1s core level spectrum shows characteristic signals of the SiC substrate, the (6√3×6√3) interface layer, and the graphene monolayer. The angle-resolved photoelectron spectroscopy (ARPES) measurement reveals the characteristic band structure of monolayer graphene. The Dirac point is shifted below the Fermi level due to electron doping from the substrate. The study concludes that the growth of epitaxial graphene on SiC(0001) in an argon atmosphere close to atmospheric pressure provides morphologically superior graphene layers compared to vacuum graphitization. The improved surface morphology is due to extensive step bunching during processing, resulting in arrays of parallel terraces up to 3 μm wide and more than 50 μm long. The terraces are essentially completely and homogeneously covered with a monolayer of graphene. The study also shows that the electronic quality of the graphene layers is high, with carrier mobilities reaching 2000 cm²/Vs at 27 K. The method is much closer to standard preparation conditions in semiconductor manufacture, allowing the use of standard CVD equipment for the fabrication of graphene layers.This study presents a method for producing high-quality, large-scale graphene layers on SiC(0001) substrates through atmospheric pressure graphitization. The process involves ex-situ graphitization of Si-terminated SiC(0001) in an argon atmosphere at about 1 bar, resulting in monolayer graphene films with significantly larger domain sizes compared to previously achievable methods. Hall measurements confirm the quality of the films, with high electronic mobilities reaching 2000 cm²/Vs at 27 K. The mobility decreases linearly with increasing temperature, likely due to electron-electron interactions. The method offers a viable route for the synthesis of uniform, wafer-size graphene layers for technological applications. However, the large-scale structural quality is currently limited by the lack of continuity and uniformity of the grown film. The study compares the results of vacuum annealing with those of ex-situ annealing under argon atmosphere, showing that the latter produces significantly improved surface morphology. The surface undergoes considerable morphological changes during graphitization, leading to a more uniform and smoother surface. The improved surface morphology is attributed to the significantly higher annealing temperature (1650°C) required for graphene formation under argon at 900 mbar compared to 1280°C in UHV. The higher temperature enhances surface diffusion, allowing the restructuring of the surface before graphene formation, leading to a more uniform and smoother surface. The study also demonstrates that the graphene layers grown under argon atmosphere exhibit high structural and electronic quality, as evidenced by LEED and photoelectron spectroscopy data. The C1s core level spectrum shows characteristic signals of the SiC substrate, the (6√3×6√3) interface layer, and the graphene monolayer. The angle-resolved photoelectron spectroscopy (ARPES) measurement reveals the characteristic band structure of monolayer graphene. The Dirac point is shifted below the Fermi level due to electron doping from the substrate. The study concludes that the growth of epitaxial graphene on SiC(0001) in an argon atmosphere close to atmospheric pressure provides morphologically superior graphene layers compared to vacuum graphitization. The improved surface morphology is due to extensive step bunching during processing, resulting in arrays of parallel terraces up to 3 μm wide and more than 50 μm long. The terraces are essentially completely and homogeneously covered with a monolayer of graphene. The study also shows that the electronic quality of the graphene layers is high, with carrier mobilities reaching 2000 cm²/Vs at 27 K. The method is much closer to standard preparation conditions in semiconductor manufacture, allowing the use of standard CVD equipment for the fabrication of graphene layers.
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[slides and audio] Towards wafer-size graphene layers by atmospheric pressure graphitization of silicon carbide.