Atomic Layer Deposition of Aluminum Phosphate Using AlMe3, PO(OMe)3, and O2 Plasma: Film Growth and Surface Reactions,The Journal of Physical Chemistry C

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Atomic Layer Deposition of Aluminum Phosphate Using AlMe3, PO(OMe)3, and O2 Plasma: Film Growth and Surface Reactions
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2020-02-24 , DOI: 10.1021/acs.jpcc.0c00301
N. Hornsveld ₁ , W. M. M. Kessels ₁ , M. Creatore ₁

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High purity, uniform, and conformal aluminum phosphate (AlP_xO_y) thin films were deposited by atomic layer deposition (ALD) between 25 and 300 °C using supercycles consisting of (i) PO(OMe)₃ dosing combined with O₂ plasma exposure and (ii) AlMe₃ dosing followed by O₂ plasma exposure. In situ spectroscopic ellipsometry and mass spectrometry were applied to demonstrate the ALD self-limiting behavior and to gain insight into the surface reactions during the precursor and coreactant exposures, respectively. Compared to earlier reported AlP_xO_y ALD studies using H₂O and O₃ as coreactants or without using coreactans, the use of an oxygen plasma generally leads to higher growth per cycle values and promotes phosphorus incorporation in the film. Specifically, when using a 1:1 PO_x:Al₂O₃ cycle ratio and a substrate temperature of 150 °C, the growth per supercycle is found to be 1.8 Å. The [P]:[Al] atomic ratio for this process is approximately 0.5 (∼AlP_0.5O_2.9) and can be tailored by changing the ratio between the two cycles or the substrate temperature. In literature reports where the same aluminum precursor was used, the [P]:[Al] atomic ratio was limited to 0.2 or a very high number of phosphorus cycles was needed in order to increase the phosphorus content. Instead, we demonstrate deposition of films with a composition close to AlPO₄ by using a 2:1 PO_x:Al₂O₃ cycle ratio. The limited incorporation of P in the film is suspected to derive from the steric hindrance of the relatively bulky phosphorus precursor. Mass spectrometry suggests that the PO(OMe)₃ precursor chemisorbs on the surface without the release of reaction products into the gas phase, whereas Al(Me)₃ already undergoes methyl ligand abstraction upon chemisorption.

中文翻译：

AlMe ₃，PO（OMe）₃和O ₂等离子体对磷酸铝的原子层沉积：膜生长和表面反应

使用由（i）PO（OMe）₃配量和O ₂等离子体组成的超循环，在25至300°C之间通过原子层沉积（ALD）沉积高纯度，均匀和共形的磷酸铝（AlP _x O _y）薄膜。暴露和（ii）AlMe ₃加药，然后进行O ₂等离子体暴露。原位光谱椭圆偏振法和质谱法分别用于证明ALD的自限行为和深入了解前体和共反应剂暴露过程中的表面反应。与先前报道的使用H ₂ O和O _3的AlP _x O _y ALD研究相比作为共反应剂或不使用共反应剂，使用氧等离子体通常会导致每个循环值更高的生长并促进磷在膜中的结合。具体地，当使用1：1的PO _x：Al ₂ O ₃循环比和基板温度为150℃时，发现每个超循环的生长为1.8。此过程的[P]：[Al]原子比约为0.5（〜AlP _0.5 O _2.9），并且可以通过更改两个循环之间的比率或基板温度进行调整。在使用相同铝前体的文献报道中，[P]：[Al]原子比限制为0.2，或者需要非常高的磷循环次数才能增加磷含量。相反，我们通过使用2：1 PO _x：Al ₂ O ₃循环比来演示沉积具有接近AlPO ₄的成分的薄膜。薄膜中磷的有限掺入被认为是由于相对庞大的磷前体的位阻所致。质谱表明PO（OMe）₃前体在表面化学吸附，而没有反应产物释放到气相中，而Al（Me）₃在化学吸附后已经经历了甲基配体的提取。

更新日期：2020-02-24

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