Graduation Year

2008

Document Type

Dissertation

Degree

Ph.D.

Degree Granting Department

Chemical Engineering

Major Professor

Stephen E. Saddow, Ph.D.

Co-Major Professor

John T. Wolan, Ph.D.

Committee Member

Norma A. Alcantar, Ph.D.

Committee Member

Andrew M. Hoff, Ph.D.

Committee Member

Ryan Toomey, Ph.D.

Committee Member

Olle Kordina, Ph.D.

Keywords

homogeneous nucleation, hydrogen chloride, computerized fluid dynamics, thermodynamic equilibrium, epitaxial layers

Abstract

This dissertation study describes the development of novel heteroepitaxial growth of 3C-SiC layers by chemical vapor deposition (CVD). It was hypothesized that chloride addition to the "traditional" propane-silane-hydrogen precursors system will enhance the deposition growth rate and improve the material quality via reduced defect density. Thermodynamic equilibrium calculations were performed to obtain a criterion for which chloride specie to select for experimentation. This included the chlorocarbons, chlorosilanes, and hydrogen chloride (HCl) chloride containing groups. This study revealed no difference in the most dominant species present in the equilibrium composition mixture between the groups considered. Therefore, HCl was the chloride specie selected to test the hypothesis.

CVD computerized fluid dynamic simulations were developed to predict the velocity, temperature and concentration profiles along the reactor. These simulations were performed using COMSOL Multiphysics and results are presented.

The development of a high-temperature (1300 °C -1390°C) 3C-SiC growth process resulted in deposition rates up to ~38 µm/h. This is the highest value reported in the literature to date for 3C-SiC heteroepitaxy. XRD FWHM values obtained varied from 220 to 1160 arcsec depending of the process growth rate or film thickness. These values are superior or comparable to those reported in the literature. It was concluded from this study that at high deposition temperatures HCl addition to the precursor chemistry had the most significant impact on the epitaxial layer growth rate.

Low-temperature (1000-1250°C) 3C-SiC growth experiments evidenced that the highest deposition rate that could be attained was ~2.5 µm/h. The best quality layer achieved in this study had a FWHM of 278 arcsec; which is comparable to values reported in the literature and to films grown at higher deposition temperatures in this study. It was concluded from this work that at lower deposition temperatures the HCl addition was more beneficial for the film quality by enhancing the surface. Surface roughness values for films grown with HCl additive were 10 times lower than for films grown without HCl.

Characterization of the epitaxial layers was carried out via Nomarski optical microscopy, FTIR, SEM, AFM, XRD and XPS.

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