Thermally Induced Structural Evolution of Silicon- and Oxygen-Containing Hydrogenated Amorphous Carbon : A Combined Spectroscopic and Molecular Dynamics Simulation Investigation

Silicon- and oxygen-containing hydrogenated amorphous carbon (a-C:H:Si:O) coatings are amorphous thin-film materials composed of hydrogenated amorphous carbon (a-C:H), doped with silicon and oxygen. Compared to a-C:H, a-C:H:Si:O exhibits much lower susceptibility to oxidative degradation and higher...

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Veröffentlicht in:Langmuir : the ACS journal of surfaces and colloids. - 1985. - 34(2018), 9 vom: 06. März, Seite 2989-2995
1. Verfasser: Mangolini, Filippo (VerfasserIn)
Weitere Verfasser: Hilbert, James, McClimon, J Brandon, Lukes, Jennifer R, Carpick, Robert W
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2018
Zugriff auf das übergeordnete Werk:Langmuir : the ACS journal of surfaces and colloids
Schlagworte:Journal Article Research Support, Non-U.S. Gov't
Beschreibung
Zusammenfassung:Silicon- and oxygen-containing hydrogenated amorphous carbon (a-C:H:Si:O) coatings are amorphous thin-film materials composed of hydrogenated amorphous carbon (a-C:H), doped with silicon and oxygen. Compared to a-C:H, a-C:H:Si:O exhibits much lower susceptibility to oxidative degradation and higher thermal stability, making a-C:H:Si:O attractive for many applications. However, the physical mechanisms for this improved behavior are not understood. Here, the thermally induced structural evolution of a-C:H:Si:O was investigated in situ by X-ray photoelectron and absorption spectroscopy, as well as molecular dynamics (MD) simulations. The spectroscopy results indicate that upon high vacuum annealing, two thermally activated processes with a Gaussian distribution of activation energies with mean value E and standard deviation σ take place in a-C:H:Si:O: (a) ordering and clustering of sp2 carbon ( E ± σ = 0.22 ± 0.08 eV) and (b) conversion of sp3- to sp2-bonded carbon ( E ± σ = 3.0 ± 1.1 eV). The experimental results are in qualitative agreement with the outcomes of MD simulations performed using a ReaxFF potential. The MD simulations also indicate that the higher thermal stability of a-C:H:Si:O compared to a-C:H (with similar fraction of sp2-bonded carbon and hydrogen content) derives from the significantly lower fraction of strained carbon-carbon sp3 bonds in a-C:H:Si:O compared to a-C:H, which are more likely to break at elevated temperatures
Beschreibung:Date Completed 10.09.2018
Date Revised 10.09.2018
published: Print-Electronic
Citation Status PubMed-not-MEDLINE
ISSN:1520-5827
DOI:10.1021/acs.langmuir.7b04266