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Phase stability and oxygen doping in the Cu-N-O system
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Inorganic Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Inorganic Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Inorganic Chemistry.
2010 (English)In: Journal of Crystal Growth, ISSN 0022-0248, E-ISSN 1873-5002, Vol. 312, no 10, 1779-1784 p.Article in journal (Refereed) Published
Abstract [en]

A growth stability diagram for the system Cu-N-O has been determined in the temperature range 250-500°C for a thermally activated CVD process, based on copper (II) hexafluoroacetylacetonate (Cu(hfac)2), NH3 and H2O. Without any addition of water only Cu3N was obtained. Addition of water introduces oxygen into the Cu3N structure to a maximum amount of 9 atomic % at a water/nitrogen molar ratio of 0.36 at 325 °C. Above this molar ratio Cu2O starts to deposit in addition to an oxygen doped Cu3N phase. Only Cu2O is deposited at a large excess of water.

XPS and Raman spectroscopy indicated that the additional oxygen in the doped Cu3N structure occupies an interstitial position with a chemical environment similar to oxygen in Cu2O. The oxygen doping of the Cu3N phase did not influence the lattice parameter which was close to the bulk parameter of 3.814 Å. The film morphology varied markedly with both deposition temperature and water concentration in the vapour during deposition.  Increasing the water concentration results in less faceted and textured films with smoother and more sphere like grains. The resistivity of the Cu3N films increased with increased oxygen content of the film and varied between 10-100 Ωcm (0 to 9 atomic% O). The optical band gap increased from 1.25 to 1.45 eV as the oxygen content increased (0 to 9 atomic %).

Place, publisher, year, edition, pages
North Holland: Elsevier , 2010. Vol. 312, no 10, 1779-1784 p.
Keyword [en]
A3. Metalorganic chemical vapour deposition, B2. copper (I) nitride, A1. Oxygen doping, A.1 Resistivity, A2. Band gap
National Category
Inorganic Chemistry
Research subject
Inorganic Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-110525DOI: 10.1016/j.jcrysgro.2010.02.025ISI: 000277483100022OAI: oai:DiVA.org:uu-110525DiVA: diva2:277187
Available from: 2009-11-16 Created: 2009-11-16 Last updated: 2017-12-12Bibliographically approved
In thesis
1. Chemical Vapour Deposition of Undoped and Oxygen Doped Copper (I) Nitride
Open this publication in new window or tab >>Chemical Vapour Deposition of Undoped and Oxygen Doped Copper (I) Nitride
2010 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

In science and technology there is a steadily increased demand of new materials and new materials production processes since they create new application areas as well as improved production technology and economy. This thesis includes development and studies of a chemical vapour deposition (CVD) process for growth of thin films of the metastable material copper nitride, Cu3N, which is a semiconductor and decomposes at around 300 oC. The combination of these properties opens for a variety of applications ranging from solar cells to sensor and information technology.

The CVD process developed is based on a metal-organic compound copper hexafluoroacetylacetonate, Cu(hfac)2 , ammonia and water and was working at about 300 oC and  5 Torr. It was found that a small amount of water in the vapour increased the growth rate considerably and that the phase content, film texture, chemical composition and morphology were strongly dependent on the deposition conditions.

In-situ oxygen doping during the CVD of Cu3N to an amount of 9 atomic % could also be accomplished by increasing the water concentration in the vapour. Oxygen doping increases the band gap of the material as well as the electrical resistivity and changes the stability. The crystal structure of Cu3N is very open and contains several sites which can be used for doping. Different spectroscopic techniques like X-ray photoelectron spectroscopy, Raman spectroscopy and near edge X-ray absorption fine structure spectroscopy were used to identify the oxygen doping site(s) in Cu3N. Besides the properties, the oxygen doping also affected the morphology and texture of the films.

By combining thin layers of different materials several properties can be optimized at the same time. It has been demonstrated in this thesis that multilayers, composed of alternating Cu3N and Cu2O layers, i.e. a metastable and a stable material, could be grown by CVD technique. However, the stacking sequence affected the texture, morphology and chemical composition. The interfaces between the different layers were sharp and no signs of decomposition of the initially deposited metastable Cu3N layer could be detected.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2010. 52 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 691
Keyword
Chemical vapour deposition, copper hexafluoroacetylacetonate, copper (I) nitride, copper (I) oxide, multilayers, oxygen doping
National Category
Organic Chemistry
Research subject
Inorganic Chemistry
Identifiers
urn:nbn:se:uu:diva-110533 (URN)978-91-554-7665-6 (ISBN)
Public defence
2010-01-08, Häggsalen, The Ångstöm Laboratory, Lägerhyddsvägen 1, Uppsala, 10:15 (English)
Opponent
Supervisors
Available from: 2009-12-09 Created: 2009-11-16 Last updated: 2009-12-09

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