Recently, TiAlSiN thin films have attracted increasing research interest due to their potential to have simultaneously enhanced hardness, thermal stability, and oxidation resistance compared with Si-free TiAlN films. Previous studies have revealed that a relatively low Si content (2.1–6.0 at.% Si) is essential for the phase stability and hardness of TiAlSiN thin films. Despite the optimum Si content for the hardness of TiAlSiN thin films being proposed, a systematical study concerning the optimum Si content for tailored phase stability, thermal stability, and oxidation resistance of TiAlSiN thin films is still missing. Here, we arc-deposited Ti1-x-zAlxSizN thin films (x = ~0.45, 0.01 ≤ z ≤ 0.08), and investigated the dependence of their structure, mechanical properties, thermal stability, and oxidation resistance on Si content. XRD analysis reveals the transformation from single-phase cubic structure for z ≤ 0.06 to a cubic-wurtzite dual-phase structure for z = 0.08. Increasing the Si content of cubic-structured Ti1-x-zAlxSizN thin films conduces a continuous increase of hardness (H) from 29.3 ± 0.5 GPa for z = 0.01 up to 37.3 ± 0.7 GPa for z = 0.06, whereas the w-AlN formation leads to a drop of H to 32.8 ± 0.6 GPa for z = 0.08. Furthermore, enhancing the Si content from z = 0.01 to z = 0.06 continuously improves film thermal stability, where the Ti0.48Al0.46Si0.06N film presents the highest hardness values within the whole studied temperature range (as-deposited, 800–1200 °C). All Ti1-x-zAlxSizN films undergo age-hardening, with peak H of 33.3 ± 1.0 GPa at 1000 °C for z = 0.01, 35.0 ± 0.6 GPa at 1100 °C for z = 0.02, 35.4 ± 0.5 GPa at 1100 °C for z = 0.03, 40.2 ± 0.7 GPa at 1200 °C for z = 0.06, and 37.8 ± 0.6 GPa at 1100 °C for z = 0.08. Additionally, the oxidation resistance of Ti1-x-zAlxSizN films at 800–1000 °C is improved with increasing Si content, due to the suppressed transformation of anatase-to-rutile TiO2 and the promoted formation of a top dense oxide scale. After oxidation at 900 °C for 15 h, the Ti0.54Al0.45Si0.01N film has been completely oxidized, whereas Ti0.53Al0.45Si0.02N, Ti0.51Al0.46Si0.03N, Ti0.48Al0.46Si0.06N and Ti0.45Al0.47Si0.08N films exhibit oxide scales of ~1.7, ~1.4, ~1.2 and ~0.9 μm, respectively. Overall, we propose z = 0.06 as the optimum Si content for the over-rounded performance of Ti1-x-zAlxSizN thin films.
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