Oxidation of heated diamond C(100):H surfaces

• Published in: Surface science Vol. 460; no. 1; pp. 74 - 90
• Main Authors: Pehrsson, Pehr E., Mercer, Thomas W.
• Format: Journal Article
• Language: English
• Published: Lausanne Elsevier B.V 20.07.2000; Amsterdam Elsevier Science; New York, NY
• Subjects: Auger electron spectroscopy; Chemistry; Cross-disciplinary physics: materials science; rheology; Diamond; Electron energy loss spectroscopy (EELS); Exact sciences and technology; General and physical chemistry; Low energy electron diffraction (LEED); Low index single crystal surfaces; Materials science; Oxidation; Oxygen; Physics; Solid-gas interface; Surface chemical reaction; Surface physical chemistry; Surface treatments; Low energy electron diffraction (LEED); Oxygen; Low index single crystal surfaces; Surface chemical reaction; Auger electron spectroscopy; Diamond; Oxidation; Electron energy loss spectroscopy (EELS); Surface reaction; Thermal activation; Gas solid desorption; Gas solid interface; LEED; Experimental study; Hydrogenation; Auger electron spectrometry; Electron energy loss spectroscopy
• ISSN: 0039-6028; 1879-2758
• DOI: 10.1016/S0039-6028(00)00495-7

This paper extends a previous study (Pehrsson and Mercer, submitted to Surf. Sci.) on unheated, hydrogenated, natural diamond (100) surfaces oxidized with thermally activated oxygen (O ∗ 2). In this paper, the oxidation is performed at substrate temperatures from T sub=24 to 670°C. The diamond surface composition and structure were then investigated with high resolution electron energy loss spectroscopy (HREELS), Auger electron spectroscopy (AES), electron loss spectroscopy (ELS) and low energy electron diffraction (LEED). The oxygen coverage ( θ) increased in two stages, as it did during oxidation at T<80°C. However, there are fundamental differences between the oxidation of nominally unheated and heated diamond surfaces. This difference is attributed to simultaneous adsorption and rapid desorption of oxygen species at higher temperatures; the desorption step is much slower without heating. The initial oxidation rates were similar regardless of the substrate temperatures, but the peak coverage ( θ) was lower at higher temperatures. For example, θ plateaued at 0.4±0.1 ML at 600°C. The lower saturation coverage is again attributed to oxygen desorption during oxidation. Consistent results were obtained on fully oxidized surfaces, which when heated in vacuum to T sub=600°C, lost ∼60% of their adsorbed oxygen. ELS revealed few CC dimers on the oxidized surfaces, and more graphitization than on unheated surfaces. Oxidation at elevated temperatures also increased the carbonyl to ether ratio, reflecting etching-induced changes in the types of surface sites. The carbonyl and C–H stretch frequencies increased with oxygen dose due to formation of higher oxidation states and/or hydrogen bonding between adjacent groups. The oxygen types did not interconvert when the oxidized surfaces were heated in vacuum. Oxygen desorption generated a much more reactive surface than heating-induced dehydrogenation of the smooth, hydrogenated surface.