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Formation of Insulating Oxide Films with Hydrolysis Reactions of Alkoxide Precursors in Supercritical Fluid CO2: Chemistry, Morphology, Characterization and Film Thickness

Published online by Cambridge University Press:  19 April 2016

Joanna S. Wang ,
Chien. M. Wai ,
Gail J. Brown ,
Scott D. Apt ,
Howard E. Smith  and
Laraba P. Kendig
Joanna S. Wang*
Affiliation:
Air Force Research Laboratory, Materials & Manufacturing Directorate, Wright-Patterson AFB, OH 45433-7707, USA
Chien. M. Wai
Affiliation:
Department of Chemistry, University of Idaho, Moscow, ID 83844, USA
Gail J. Brown
Affiliation:
Air Force Research Laboratory, Materials & Manufacturing Directorate, Wright-Patterson AFB, OH 45433-7707, USA
Scott D. Apt
Affiliation:
Air Force Research Laboratory, Materials & Manufacturing Directorate, Wright-Patterson AFB, OH 45433-7707, USA
Howard E. Smith
Affiliation:
Air Force Research Laboratory, Materials & Manufacturing Directorate, Wright-Patterson AFB, OH 45433-7707, USA
Laraba P. Kendig
Affiliation:
Air Force Research Laboratory, Materials & Manufacturing Directorate, Wright-Patterson AFB, OH 45433-7707, USA
*
*(Email: [email protected])
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Abstract

Insulating silicon dioxide (SiO2) films can be produced by hydrolysis of metal alkoxide tetraethylorthosilicate (TEOS) in the presence of an acid catalyst in supercritical fluid CO2 (sc-CO2). In this study, SiO2 films are formed on different substrates using TEOS as a source of silicon, and acetic acid (HAc) as a catalyst. Water required for the hydrolysis reaction is from in situ generation of esterification and condensation reactions involving HAc and the alcohol produced. The acid catalyzed deposition reaction actually starts at room temperature but produces decent films in sc-CO2 at moderately high temperatures (e.g. 50 °C). Supercritical fluid CO2 is known to have near zero surface tension and provides an ideal medium for fabrication of SiO2 films. Formation of SiO2 films via hydrolysis reaction in sc-CO2 is more rapid compared to the traditional hydrolysis reaction at room temperature. In general, metal alkoxide hydrolysis reactions carried out in a closed sc-CO2 system is not affected by moisture in air compared with traditional open-air hydrolysis systems. Using sc-CO2 as a reaction medium can eliminate undesirable organic solvents utilized in traditional alkoxide hydrolysis reactions.

X-ray diffraction (XRD) and electron diffraction (ED) measurements demonstrated that the SiO2 films produced are amorphous. Energy dispersive spectroscopy (EDS), attenuated total reflectance-Fourier transform infrared (ATR-FTIR) and X-ray photoelectron (XPS) spectroscopy show elemental compositions of the films formed on the substrate surfaces to be SiO2. Film thickness formation by controlling the amount of the catalyst is discussed.

Keywords

thin filmamorphousnanostructure
Type
Articles
Information
MRS Advances , Volume 1 , Issue 37: Nanotechnology , 2016 , pp. 2591 - 2596
Copyright
Copyright © Materials Research Society 2016 

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References

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