Effects of Ambient Oxygen on Initial Stage of Carbon Nanotube Formation in Surface Decomposition of 6H-SiC(000-1)

Abstract

It has been reported that carbon nanotubes (CNTs) were formed through the decomposition of SiC(000-1) surfaces by heating in a vacuum. By this growth technique, well aligned zigzag-type CNTs can be selectively formed without any catalysts and the diameters of the CNTs are fairly uniform. Moreover, this growth technique has an advantage in fabrication of CNT devices, since CNTs grow into the inside of SiC, facilitating the application of semiconductor process. So far, we have reported that ambient oxygen enhances the CNT growth rate [1]. However, the optimum oxygen pressure has never been investigated enough. It has also been reported that SiO2 layer is formed on SiC surface after annealing under high oxygen pressure [2]. In this study, we investigated the relation between surface oxide formation and CNT growth under various annealing conditions. After HF etching, 6H-SiC(000-1) (Carbon-face) samples were introduced into an ultra-high vacuum (UHV) chamber and annealed at various temperatures between 800 and 1250°C. During the annealing, oxygen partial pressure was controlled by supply of oxygen gas. The oxygen pressure was set between 10-4 and 1 Pa. For comparison, we also annealed several samples under UHV (10-6 Pa). Scanning tunneling microscopy (STM) observation and X-ray photoelectron spectroscopy (XPS) measurements were carried out to analyze their surface structures and chemical species. It was observed that the surface decomposition of SiC had occurred after annealing at 800°C under UHV, and carbon nanocaps were formed on the SiC surface at 1200°C, which subsequently transformed into CNTs. When oxygen pressure was below 10-2 Pa, the nanocap formation was observed between 1150 and 1200°C irrespective of oxygen pressure. However, at 1 Pa of oxygen pressure, SiO2 layer was observed on the SiC surface after annealing at 1200°C and no carbon nanocaps were observed. These results indicate that it is necessary to anneal SiC below 1 Pa to form CNT, although the presence of oxygen enhances CNT formation below 10-3 Pa. The boundary between the active oxidation and the passive oxidation in SiC oxidation estimated from our results was well consistent with previous studies for SiC oxidation under higher oxygen pressure (>1 Pa)[2]. From our results, in order to grow CNT effectively, it is important to minutely control oxygen pressure.