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Low-temperature alpha-alumina thin film growth: ab initio studies of Al adatom surface migration
Linköping University, Department of Physics, Chemistry and Biology, Plasma and Coating Physics . Linköping University, The Institute of Technology.
Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics . Linköping University, The Institute of Technology.
Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, The Institute of Technology.
Linköping University, Department of Physics, Chemistry and Biology, Plasma and Coating Physics . Linköping University, The Institute of Technology.ORCID iD: 0000-0002-1744-7322
2009 (English)In: JOURNAL OF PHYSICS D-APPLIED PHYSICS, ISSN 0022-3727, Vol. 42, no 12, 125302- p.Article in journal (Refereed) Published
Abstract [en]

Investigations of activation energy barriers for Al surface hopping on alpha-Al2O3 (0 0 0 1) surfaces have been carried out by means of first-principles density functional theory calculations and the nudged elastic band method. Results show that surface diffusion on the (most stable) Al-terminated surface is relatively fast with an energy barrier of 0.75 eV, whereas Al hopping on the O-terminated surface is slower, with barriers for jumps from the two metastable positions existing on this surface to the stable site of 0.31 and 0.99 eV. Based on this study and on the literature, the governing mechanisms during low-temperature alpha-alumina thin film growth are summarized and discussed. Our results support suggestions made in some previous experimental studies, pointing out that limited surface diffusivity is not the main obstacle for alpha-alumina growth at low-to-moderate temperatures, and that other effects should primarily be considered when designing novel processes for low-temperature alpha-alumina deposition.

Place, publisher, year, edition, pages
2009. Vol. 42, no 12, 125302- p.
National Category
Natural Sciences
Identifiers
URN: urn:nbn:se:liu:diva-19393DOI: 10.1088/0022-3727/42/12/125302OAI: oai:DiVA.org:liu-19393DiVA: diva2:224875
Note
Original Publication: Erik Wallin, Peter Münger, Valeriu Chirita and Ulf Helmersson, Low-temperature alpha-alumina thin film growth: ab initio studies of Al adatom surface migration, 2009, JOURNAL OF PHYSICS D-APPLIED PHYSICS, (42), 12, 125302. http://dx.doi.org/10.1088/0022-3727/42/12/125302 Copyright: Iop Publishing Ltd http://www.iop.org/ Available from: 2009-06-29 Created: 2009-06-22 Last updated: 2013-10-30Bibliographically approved
In thesis
1. Alumina Thin Films: From Computer Calculations to Cutting Tools
Open this publication in new window or tab >>Alumina Thin Films: From Computer Calculations to Cutting Tools
2008 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The work presented in this thesis deals with experimental and theoretical studies related to alumina thin films. Alumina, Al2O3, is a polymorphic material utilized in a variety of applications, e.g., in the form of thin films. However, controlling thin film growth of this material, in particular at low substrate temperatures, is not straightforward. The aim of this work is to increase the understanding of the basic mechanisms governing alumina growth and to investigate novel ways of synthesizing alumina coatings. The thesis can be divided into two main parts, where the first part deals with fundamental studies of mechanisms affecting alumina growth and the second part with more application-oriented studies of high power impulse magnetron sputter (HiPIMS) deposition of the material.

In the first part, it was shown that the thermodynamically stable α phase, which normally is synthesized at substrate temperatures of around 1000 °C, can be grown using reactive sputtering at a substrate temperature of merely 500 °C by controlling the nucleation surface. This was done by predepositing a Cr2O3 nucleation layer. Moreover, it was found that an additional requirement for the formation of the α phase is that the depositions are carried out at low enough total pressure and high enough oxygen partial pressure. Based on these observations, it was concluded that energetic bombardment, plausibly originating from energetic oxygen, is necessary for the formation of α-alumina (in addition to the effect of the chromia nucleation layer). Moreover, the effects of residual water on the growth of crystalline films were investigated by varying the partial pressure of water in the ultra high vacuum (UHV) chamber. Films deposited onto chromia nucleation layers exhibited a columnar structure and consisted of crystalline α-alumina if deposited under UHV conditions. However, as water to a partial pressure of 1*10-5 Torr was introduced, the columnar α-alumina growth was disrupted. Instead, a microstructure consisting of small, equiaxed grains was formed, and the γ-alumina content was found to increase with increasing film thickness.

To gain a better understanding of the atomistic processes occurring on the surface, density functional theory based computational studies of adsorption and diffusion of Al, O, AlO, and O2 on different α-alumina (0001) surfaces were also performed. The results give possible reasons for the difficulties in growing the α phase at low temperatures through the identification of several metastable adsorption sites and also show how adsorbed hydrogen might inhibit further growth of α-alumina crystallites. In addition, it was shown that the Al surface diffusion activation energies are unexpectedly low, suggesting that limited surface diffusivity is not the main obstacle for low-temperature α-alumina growth. Instead, it is suggested to be more important to find ways of reducing the amount of impurities, especially hydrogen, in the process and to facilitate α-alumina nucleation when designing new processes for low-temperature deposition of α-alumina.

In the second part of the thesis, reactive HiPIMS deposition of alumina was studied. In HiPIMS, a high-density plasma is created by applying very high power to the sputtering magnetron at a low duty cycle. It was found, both from experiments and modeling, that the use of HiPIMS drastically influences the characteristics of the reactive sputtering process, causing reduced target poisoning and thereby reduced or eliminated hysteresis effects and relatively high deposition rates of stoichiometric alumina films. This is not only of importance for alumina growth, but for reactive sputter deposition in general, where hysteresis effects and loss of deposition rate pose a substantial problem. Moreover, it was found that the energetic and ionized deposition flux in the HiPIMS discharge can be used to lower the deposition temperature of α-alumina. Coatings predominantly consisting of the α phase were grown at temperatures as low as 650 °C directly onto cemented carbide substrates without the use of nucleation layers. Such coatings were also deposited onto cutting inserts and were tested in a steel turning application. The coatings were found to increase the crater wear resistance compared to a benchmark TiAlN coating, and the process consequently shows great potential for further development towards industrial applications.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2008. 59 p.
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1221
Keyword
Alumina, thin films, coatings, sputtering, density functional theory, high power impulse magnetron sputtering, HIPIMS
National Category
Other Engineering and Technologies not elsewhere specified Manufacturing, Surface and Joining Technology Condensed Matter Physics
Identifiers
urn:nbn:se:liu:diva-15360 (URN)978-91-7393-769-6 (ISBN)
Public defence
2008-11-27, Planck, Physics building, Campus Valla, Linköping University, Linköping, 10:15 (English)
Opponent
Supervisors
Available from: 2008-11-05 Created: 2008-11-05 Last updated: 2013-10-30Bibliographically approved

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Wallin, ErikMünger, PeterChirita, ValeriuHelmersson, Ulf

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