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In situ transmission infrared spectroscopy of high-k oxide atomic layer deposition onto silicon surfaces
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In situ transmission infrared spectroscopy of high-k oxide atomic layer deposition onto silicon surfaces
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Ho
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Ming-Tsung
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Ming-Tsung Ho
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Yves
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Advisory Committee
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Yves J. Chabal
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Langreth
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David
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David C. Langreth
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Garfunkel
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Eric
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Advisory Committee
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Eric Garfunkel
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Watts
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Terence
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Advisory Committee
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Terence L. Watts
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Mann
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Adrian
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Advisory Committee
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Adrian M. Mann
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Rutgers University
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Graduate School - New Brunswick
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theses
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2008
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2008-01
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English
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electronic
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text/xml
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xxiii, 165 pages
Abstract
Ultra-thin aluminum oxide (Al2O3 ) and hafnium oxide (HfO2) layers have been grown by atomic layer deposition (ALD) using tri-methyl-aluminum (TMA) and tetrakis-ethyl-methyl-amino-hafnium (TEMAH) respectively with heavy water (D2O) as the oxidizing agent. Several different silicon surfaces were used as substrates such as hydrogen terminated silicon (H/Si), SC2 (or RCA 2) cleaned native silicon oxide (SiO2/Si), and silicon (oxy)nitride. In-situ transmission Fourier transform infrared spectroscopy (FTIR) has been adopted for the study of the growth mechanisms during ALD of these films.
The vibrational spectra of gas phase TEMAH and its reaction byproducts with oxidants have also been investigated. Density functional theory (DFT) normal mode calculations show a good agreement with the experimental data when it is combined with linear wave-number scaling method and Fermi resonance mechanism. Ether (-C-O-C-) and tertiary alkylamine (N(R1R2R3)) compounds are the two most dominant products of TEMAH reacting with oxygen gas and water. When ozone is used as the oxidant, gas phase CH2O, CH3NO2, CH3-N=C=O and other compounds containing -(C=O)- and --C- O-C- (or --O-C-) segments are observed.
With substrate temperatures less than 400oC and 300oC for TMA and TEMAH respectively, Al oxide and Hf oxide ALD can be appropriately performed on silicon surfaces. Thin silicon (oxy)nitride thermally grown in ammonia on silicon substrate can significantly reduce silicon oxide interlayer formation during ALD and post-deposition annealing. The crystallization temperature of amorphous ALD grown HfO2 on nitridized silicon is 600oC, which is 100oC higher than on the other silicon surfaces.
When HfO2 is grown on H/Si(111) at 100oC deposition temperature, minimum 5 -- 10 ALD cycles are required for the full surface coverage. The steric effect can be seen by the evolution of the H-Si stretching mode at 2083 cm-1. The observed red shift of H-Si stretching to ~ 2060 cm-1 can be caused by Si-H...Hf interactions or by the dielectric screening effect of as-grown high-κ moiety. A summary of local bonding models with vibrational mode assignments of the adsorbed TMA and TEMAH on silicon surfaces is presented based on the analysis of the substructure of silicate interfacial band at 900 -- 1100 cm-1.
The vibrational spectra of gas phase TEMAH and its reaction byproducts with oxidants have also been investigated. Density functional theory (DFT) normal mode calculations show a good agreement with the experimental data when it is combined with linear wave-number scaling method and Fermi resonance mechanism. Ether (-C-O-C-) and tertiary alkylamine (N(R1R2R3)) compounds are the two most dominant products of TEMAH reacting with oxygen gas and water. When ozone is used as the oxidant, gas phase CH2O, CH3NO2, CH3-N=C=O and other compounds containing -(C=O)- and --C- O-C- (or --O-C-) segments are observed.
With substrate temperatures less than 400oC and 300oC for TMA and TEMAH respectively, Al oxide and Hf oxide ALD can be appropriately performed on silicon surfaces. Thin silicon (oxy)nitride thermally grown in ammonia on silicon substrate can significantly reduce silicon oxide interlayer formation during ALD and post-deposition annealing. The crystallization temperature of amorphous ALD grown HfO2 on nitridized silicon is 600oC, which is 100oC higher than on the other silicon surfaces.
When HfO2 is grown on H/Si(111) at 100oC deposition temperature, minimum 5 -- 10 ALD cycles are required for the full surface coverage. The steric effect can be seen by the evolution of the H-Si stretching mode at 2083 cm-1. The observed red shift of H-Si stretching to ~ 2060 cm-1 can be caused by Si-H...Hf interactions or by the dielectric screening effect of as-grown high-κ moiety. A summary of local bonding models with vibrational mode assignments of the adsorbed TMA and TEMAH on silicon surfaces is presented based on the analysis of the substructure of silicate interfacial band at 900 -- 1100 cm-1.
Note
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Ph.D.
Note
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Includes bibliographical references (p. 161-164).
Subject
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Topic
Physics and Astronomy
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Topic
Semiconductors
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Topic
Integrated circuits
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(ID = SUBJ4);
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Topic
Thin films
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Graduate School - New Brunswick Electronic Theses and Dissertations
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http://hdl.rutgers.edu/1782.2/rucore10001600001.ETD.17137
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doi:10.7282/T39C6XSF
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ETD doctoral
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Open
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Ming-Tsung Ho
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Rutgers University. Graduate School - New Brunswick
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Non-exclusive ETD license
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I hereby grant to the Rutgers University Libraries and to my school the non-exclusive right to archive, reproduce and distribute my thesis or dissertation, in whole or in part, and/or my abstract, in whole or in part, in and from an electronic format, subject to the release date subsequently stipulated in this submittal form and approved by my school. I represent and stipulate that the thesis or dissertation and its abstract are my original work, that they do not infringe or violate any rights of others, and that I make these grants as the sole owner of the rights to my thesis or dissertation and its abstract. I represent that I have obtained written permissions, when necessary, from the owner(s) of each third party copyrighted matter to be included in my thesis or dissertation and will supply copies of such upon request by my school. I acknowledge that RU ETD and my school will not distribute my thesis or dissertation or its abstract if, in their reasonable judgment, they believe all such rights have not been secured. I acknowledge that I retain ownership rights to the copyright of my work. I also retain the right to use all or part of this thesis or dissertation in future works, such as articles or books.
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