Stranski-Krastanov and Volmer-Weber CVD Growth Regimes To Control the Stacking Order in Bilayer Graphene.
Aside from unusual properties of monolayer graphene, bilayer has been shown to have even more interesting physics, in particular allowing bandgap opening with dual gating for proper interlayer symmetry. Such properties, promising for device applications, ignited significant interest in understanding and controlling the growth of bilayer graphene. Here we systematically investigate a broad set of flow rates and relative gas ratio of CH4to H2in atmospheric pressure chemical vapor deposition of multilayered graphene. Two very different growth windows are identified. For relatively high CH4to H2ratios, graphene growth is relatively rapid with an initial first full layer forming in seconds upon which new graphene flakes nucleate then grow on top of the first layer. The stacking of these flakes versus the initial graphene layer is mostly turbostratic. This growth mode can be likened to Stranski-Krastanov growth. With relatively low CH4to H2ratios, growth rates are reduced due to a lower carbon supply rate. In addition bi-, tri-, and few-layer flakes form directly over the Cu substrate as individual islands. Etching studies show that in this growth mode subsequent layers form beneath the first layer presumably through carbon radical intercalation. This growth mode is similar to that found with Volmer-Weber growth and was shown to produce highly oriented AB-stacked materials. These systematic studies provide new insight into bilayer graphene formation and define the synthetic range where gapped bilayer graphene can be reliably produced.
College of Physics, Optoelectronics and Energy & Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow University , Suzhou 215006, China.|Centre of Polymer and Carbon Materials, Polish Academy of Sciences , M. Curie-Sklodowskiej 34, Zabrze 41-819, Poland.|Department of Energy Science, Department of Physics, Sungkyunkwan University , Suwon 16419, Republic of Korea.
Huy Q
HQ
Ta
Center for Integrated Nanostructure Physics, Institute for Basic Science, Sungkyunkwan University , Suwon 16419, Republic of Korea.
David J
DJ
Perello
Center for Integrated Nanostructure Physics, Institute for Basic Science, Sungkyunkwan University , Suwon 16419, Republic of Korea.
Dinh Loc
DL
Duong
Center for Integrated Nanostructure Physics, Institute for Basic Science, Sungkyunkwan University , Suwon 16419, Republic of Korea.
Gang Hee
GH
Han
Department of Physics, University of Oslo , Blindern, P.O. Box 1048, 0316 Oslo, Norway.
Sandeep
S
Gorantla
Center for Integrated Nanostructure Physics, Institute for Basic Science, Sungkyunkwan University , Suwon 16419, Republic of Korea.
Van Luan
VL
Nguyen
Centre of Polymer and Carbon Materials, Polish Academy of Sciences , M. Curie-Sklodowskiej 34, Zabrze 41-819, Poland.|IFW Dresden, P.O. Box 270116, D-01171 Dresden, Germany.
Alicja
A
Bachmatiuk
Department of Physics and Center for Advanced Materials and Nanotechnology, Lehigh University , Bethlehem, Pennsylvania 18015, United States.
Slava V
SV
Rotkin
Center for Integrated Nanostructure Physics, Institute for Basic Science, Sungkyunkwan University , Suwon 16419, Republic of Korea.|Department of Energy Science, Department of Physics, Sungkyunkwan University , Suwon 16419, Republic of Korea.
Young Hee
YH
Lee
College of Physics, Optoelectronics and Energy & Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow University , Suzhou 215006, China.|Centre of Polymer and Carbon Materials, Polish Academy of Sciences , M. Curie-Sklodowskiej 34, Zabrze 41-819, Poland.|IFW Dresden, P.O. Box 270116, D-01171 Dresden, Germany.
Mark H
MH
Rümmeli
Bilayer graphene; growth mechanism; hydrogen role; stacking control; stacking order