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Ti2Al(O,N) formation by solid state reaction between substoichiometric TiN thin films and Al2O3(0001) substrates
Linköpings universitet, Institutionen för fysik, kemi och biologi, Tunnfilmsfysik. Linköpings universitet, Tekniska högskolan.ORCID-id: 0000-0001-9140-6724
Linköpings universitet, Institutionen för fysik, kemi och biologi, Tunnfilmsfysik. Linköpings universitet, Tekniska högskolan.
Linköpings universitet, Institutionen för fysik, kemi och biologi, Tunnfilmsfysik. Linköpings universitet, Tekniska högskolan.
Linköpings universitet, Institutionen för fysik, kemi och biologi, Tunnfilmsfysik. Linköpings universitet, Tekniska högskolan.ORCID-id: 0000-0002-2837-3656
2011 (engelsk)Inngår i: Thin Solid Films, ISSN 0040-6090, E-ISSN 1879-2731, Vol. 519, nr 8, s. 2421-2425Artikkel i tidsskrift (Fagfellevurdert) Published
Abstract [en]

Titanium nitride TiNx (0.1 ≤ x ≤ 1) thin films were deposited onto Al2O3(0001) substrates using reactive magnetron sputtering at substrate temperatures (Ts) ranging from 800 ºC to 1000 ºC and N2 partial pressures (pN2) between 0.1 and 1.0 mTorr. It is found that Al and O from the substrates diffuse into the substoichiometric TiNx films during deposition. Solid state reactions between the film and substrate result in the formation of Ti2O and Ti3Al domains at low N2 partial pressures, while for increasing pN2, the Ti2AlN MAX phase nucleates and grows together with TiNx. Depositions at increasingly stoichiometric conditions result in a decreasing incorporation of the substrate species into the growing film. Eventually, a stoichiometric deposition gives a stable TiN(111) || Al2O3(0001) structure without the incorporation of substrate species. Growth at Ts 1000 ºC yields Ti2AlN(0001), leading to a reduced incorporation of substrate species compared to films grown at 900 ºC, but contains also Ti2AlN(101ɸ3) grains. Finally, the Ti2AlN domains incorporate O, likely on the N site, such that a MAX phase oxynitride Ti2Al(O,N) is formed. The results were obtained by a combination of structural methods, including X-ray diffraction (XRD) and (scanning) transmission electron microscopy ((S)TEM), together with spectroscopy methods, which comprise elastic recoil detection analysis (ERDA), energy dispersive X-ray spectroscopy (EDX), and electron energy loss spectroscopy (EELS).

sted, utgiver, år, opplag, sider
Elsevier , 2011. Vol. 519, nr 8, s. 2421-2425
HSV kategori
Identifikatorer
URN: urn:nbn:se:liu:diva-56273DOI: 10.1016/j.tsf.2010.12.002ISI: 000287631500007OAI: oai:DiVA.org:liu-56273DiVA, id: diva2:318045
Merknad
Original Publication: P. O. Å. Persson, Carina Höglund, Jens Birch and Lars Hultman, Ti2Al(O,N) formation by solid state reaction between substoichiometric TiN thin films and Al2O3(0001) substrates, 2011, Thin Solid Films, (519), 2421-2425. http://dx.doi.org/10.1016/j.tsf.2010.12.002 Copyright: Elsevier Science B.V., Amsterdam. http://www.elsevier.com/ Tilgjengelig fra: 2010-05-06 Laget: 2010-05-06 Sist oppdatert: 2017-12-12
Inngår i avhandling
1. Growth and Phase Stability Studies of Epitaxial Sc-Al-N and Ti-Al-N Thin Films
Åpne denne publikasjonen i ny fane eller vindu >>Growth and Phase Stability Studies of Epitaxial Sc-Al-N and Ti-Al-N Thin Films
2010 (engelsk)Doktoravhandling, med artikler (Annet vitenskapelig)
Abstract [en]

¨This Thesis treats the growth and characterization of ternary transition metal nitride thin films. The aim is to probe deep into the Ti-Al-N system and to explore novel Sc-Al-N compounds. Thin films were epitaxially grown by reactive dual magnetron sputtering from elemental targets onto single-crystal substrates. Ion beam analyses were used for compositional analysis and depth profiling. Different X-ray diffraction techniques were employed, ex situ using Cu radiation and in situ during deposition using synchrotron radiation, to achieve information about phases, texture, and thickness of films, and to follow roughness evolution of layers during and after growth. Transmission electron microscopy was used for overview and lattice imaging, and to obtain lattice structure information by electron diffraction.

In the Sc-Al-N system, the perovskite Sc3AlN was for the first time synthesized as a thin film and in single phase, with a unit cell of 4.40 Å. The hardness was found to be 14.2 GPa, the elastic modulus 21 GPa, and the room temperature resistivity 41.2 μΩcm. Cubic solid solutions of Sc1-xAlxN can be synthesized with AlN molar fraction up to ~60%. Higher AlN contents yield three different epitaxial relations to ScN(111), namely, #1 Sc1-xAlxN(0001) || ScN(111) with Sc1-xAlxN[11210] || ScN[110], #2 Sc1-xAlxN(1011) || ScN(110) with Sc1-xAlxN[1210] || ScN[110], and #3 Sc1-xAlxN(1011) || ScN(113). An in situ deposition and annealing study of cubic Sc0.57Al0.43N films showed volume induced phase separation into ScN and wurtzite structure AlN, via nucleation and growth at the domain boundaries. The first indications for phase separation are visible at 1000 °C, and the topotaxial relationship between the binaries after phase separation is AlN(0001) || ScN(001) and AlN<01ɸ10> || ScN <1ɸ10>. This is compared with Ti1-xAlxN, for which an electronic structure driving force leads to spinodal decomposition into isostructural TiN and AlN already at 800 °C. First principles calculations explain the results on a fundamental physics level. Up to ~22% ScN can under the employed deposition conditions be dissolved into wurtzite Sc1-xAlxN films, while retaining a single-crystal structure and with lattice parameters matching calculated values.

In the Ti-Al-N system, the Ti2AlN phase was synthesized epitaxially by solid state reaction during interdiffusion between sequentially deposited layers of AlN(0001) and Ti(0001). When annealing the sample, N and Al diffused into the Ti layer, forming Ti3AlN(111) at 400 ºC and Ti2AlN(0001) at 500 ºC. The Ti2AlN formation temperature is 175 ºC lower than earlier reported results. Another way of forming Ti2AlN phase is by depositing understoichiometric TiNx at 800 °C onto Al2O3(0001). An epitaxial Ti2Al(O,N) (0001) oxynitride forms close to the interface between film and substrate through a solid state reaction. Ti4AlN3 was, however, not possible to synthesize when depositing films with a Ti:Al:N ratio of 4:1:3 due to competing reactions. A substrate temperature of 600 ºC yielded an irregularly stacked Tin+1AlNn layered structure because of the low mobility of Al ad-atoms. An increased temperature led to Al deficiency due to outdiffusion of Al atoms, and formation of the Ti2AlN phase and a Ti1-xAlxN cubic solid solution.

sted, utgiver, år, opplag, sider
Linköping: Linköping University Electronic Press, 2010. s. 98
Serie
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1314
HSV kategori
Identifikatorer
urn:nbn:se:liu:diva-56274 (URN)978-91-7393-391-9 (ISBN)
Disputas
2010-05-28, Visionen, Hus B, ingång 27, Campus Valla, Linköpings universitet, Linköping, 09:15 (engelsk)
Opponent
Veileder
Tilgjengelig fra: 2010-05-06 Laget: 2010-05-06 Sist oppdatert: 2016-08-31bibliografisk kontrollert

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