Oxygen incorporated during deposition determines the crystallinity of magnetron-sputtered Ta3N5 films

• Published in: Thin solid films 2019-09, Vol.685, p.204-209
• Main Authors: Rudolph, M., Vickridge, I., Foy, E., Alvarez, J., Kleider, J.-P., Stanescu, D., Magnan, H., Herlin-Boime, N., Bouchet-Fabre, B., Minea, T., Hugon, M.-C.
• Format: Article
• Language: English
• Subjects: Chemical Sciences; Condensed Matter; Material chemistry; Materials Science; Physics; Plasma Physics; Reactive magnetron sputtering; Tantalum oxynitride; Tantalum(V) nitride; Transition metal nitride
• ISSN: 0040-6090; 1879-2731
• DOI: 10.1016/j.tsf.2019.06.031

Ta3N5 belongs to the group of transition metal nitrides with the cation in a high oxidation state. These are typically challenging to synthesize owing to the low reactivity of nitrogen. This applies similarly to Ta3N5 that crystallizes only in the presence of oxygen during synthesis. Typical preparation methods are ammonolysis of oxidized Ta or magnetron sputtering of a Ta target in an atmosphere of Ar, N2 and O2. However, the material typically obtained by either synthesis method is of varying degrees of crystallinity and the key parameter affecting the crystallinity remains elusive. In this study, we examine the role of oxygen for the crystallinity of Ta3N5 samples by studying. Thin film samples prepared by magnetron sputtering reveal that oxygen is indeed the central driver for Ta3N5 crystallinity. While little oxygen in the films yields the metallic δ-TaN phase, excess oxygen results in low crystallinity Ta3N5 or Ta-O-N films. Ta3N5 samples with a high degree of crystallinity are obtained by limiting the oxygen supply to the sample during the deposition. A comparison with other studies suggests a fundamental oxygen incorporation limit above which the crystallinity of Ta3N5 is compromised. The most crystalline sample from this study contains 4.4 at.% of oxygen. It is grown onto a Si(100) substrate, covered with a 30 nm-thick metallic diffusion layer. For this sample, we observe Ta3N5 grains between 80 and 120 nm in size. •The degree of crystallinity of Ta3N5 thin films is determined by its oxygen content.•A fundamental limit of oxygen incorporation in Ta3N5 crystalline films is suggested.•Ta interlayer between Si substrate and Ta3N5 promotes crystallization.•Large Ta3N5 grain sizes between 80 and 120 nm are obtained.