<br>X 射线光电子能谱研究结晶和非晶氧化铝氮化形成的氮的化学键,RSC Advances

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X 射线光电子能谱研究结晶和非晶氧化铝氮化形成的氮的化学键
RSC Advances ( IF 3.9 ) Pub Date : 2020-7-28 , DOI: 10.1039/d0ra05104g
K Lawniczak-Jablonska ₁ , Z R Zytkiewicz ₁ , S Gieraltowska ₁ , M Sobanska ₁ , P Kuzmiuk ₁ , K Klosek ₁

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人们已经做出了许多努力来优化晶体蓝宝石（c-Al ₂ O ₃ ）衬底的氮化，而对非晶氧化铝层（a-AlO _x ）的氮化却很少关注。因此，需要对非晶氧化铝薄膜与氮物质的反应进行广泛分析，以阐明氮掺入此类层的机制并控制其性能。在这项工作中，X 射线光电子能谱用于确定氮等离子体处理 c-Al ₂ O ₃和通过原子层沉积在硅和蓝宝石衬底上生长的 15 nm 厚 a-AlO _x层而形成的氮的化学态。结果表明，c-Al ₂ O ₃和a-AlO _x样品的氮化过程显着不同，我们将其与两种材料的初始化学计量相关联。在蓝宝石表面发现了 O 空位，这是通过氮有限扩散取代氧形成 AlN 型键合所必需的。这个过程很缓慢并且涉及氮氧化物AlN-O的形成。 80 分钟氮化后，仅掺入了约 3.4 at% 的 N。相反，在a-AlO _x层中，氮化之前存在Al空位。这开辟了一条新的、更有效的氮掺入途径，即通过在缺阳离子晶格中积累氮并形成 Al(NO _y ) _x相，然后形成 AlN 和 AlN-O。正如实际观察到的那样，这种情况预测 a-AlO _x中的氮掺入比 c-Al ₂ O ₃更有效。这也解释了我们的发现：由于蓝宝石衬底提供了氧，硅上的 a-AlO _x中的氮含量比蓝宝石上的氮含量要多。

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Chemical bonding of nitrogen formed by nitridation of crystalline and amorphous aluminum oxide studied by X-ray photoelectron spectroscopy

Numerous efforts have already been made to optimize nitridation of crystalline sapphire (c-Al₂O₃) substrates whereas very little attention has been paid to nitridation of amorphous aluminum oxide layers (a-AlO_x). An extensive analysis of the reaction of amorphous aluminum oxide films with nitrogen species is thus needed to clarify the mechanisms of nitrogen incorporation into such layers and to control their properties. In this work X-ray photoelectron spectroscopy was used to determine the chemical state of nitrogen formed by nitrogen plasma treatment of c-Al₂O₃ and 15 nm thick a-AlO_x layers grown by atomic layer deposition on Si and sapphire substrates. The results show that the nitridation proceeds significantly different for c-Al₂O₃ and a-AlO_x samples, which we correlate with the initial stoichiometry of both materials. At the surface of sapphire O vacancies were found, which are necessary for the formation of AlN-type bonding via diffusion limited replacement of oxygen by nitrogen. This process was slow and involved formation of oxinitride AlN–O. After 80 min of nitridation only ∼3.4 at% of N was incorporated. In contrast, in a-AlO_x layers Al vacancies were present before nitridation. This opened a new, more effective path for nitrogen incorporation via accumulation of N in the cation-deficient lattice and creation of the Al(NO_y)_x phase, followed by AlN and AlN–O formation. This scenario predicts more effective nitrogen incorporation into a-AlO_x than c-Al₂O₃, as indeed observed. It also explains our finding that more N was incorporated into a-AlO_x on Si than on sapphire due to supply of oxygen from the sapphire substrate.

更新日期：2020-07-28

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