A Three-Step Atomic Layer Deposition Process for SiN x Using Si2 Cl6 , CH3 NH2 , and N2 Plasma

ACS Applied Materials & Interfaces
Rafaiel A OvanesyanSumit Agarwal

Abstract

We report a novel three-step SiN x atomic layer deposition (ALD) process using Si2Cl6, CH3NH2, and N2 plasma. In a two-step process, nonhydrogenated chlorosilanes such as Si2Cl6 with N2 plasmas lead to poor-quality SiN x films that oxidize rapidly. The intermediate CH3NH2 step was therefore introduced in the ALD cycle to replace the NH3 plasma step with a N2 plasma, while using Si2Cl6 as the Si precursor. This three-step process lowers the atomic H content and improves the film conformality on high-aspect-ratio nanostructures as Si-N-Si bonds are formed during a thermal CH3NH2 step in addition to the N2 plasma step. During ALD, the reactive surface sites were monitored using in situ surface infrared spectroscopy. Our infrared spectra show that, on the post-N2 plasma-treated SiN x surface, Si2Cl6 reacts primarily with the surface -NH2 species to form surface -SiCl x ( x = 1, 2, or 3) bonds, which are the reactive sites during the CH3NH2 cycle. In the N2 plasma step, reactive -NH2 surface species are created because of the surface H available from the -CH3 groups. At 400 °C, the SiN x films have a growth per cycle of ∼0.9 Å with ∼12 atomic percent H. The films grown on high-aspect-ratio nanostructures have a conformality of ∼90%.

References

Feb 20, 1997·The Astrophysical Journal·M P BernsteinL J Allamandola
Dec 2, 2009·Chemical Reviews·Steven M George
Sep 3, 2010·Langmuir : the ACS Journal of Surfaces and Colloids·Vikrant R RaiSumit Agarwal
Mar 1, 2012·Journal of the American Chemical Society·Didier BéguéCurt Wentrup
May 1, 2015·ACS Applied Materials & Interfaces·Rafaiel A OvanesyanSumit Agarwal
Aug 26, 2015·ACS Applied Materials & Interfaces·Harm C M KnoopsWilhelmus M M Kessels
Sep 24, 2015·ACS Applied Materials & Interfaces·Anne-Marije AndringaMariadriana Creatore
Jul 23, 2016·ACS Applied Materials & Interfaces·Jae-Min ParkSang-Ick Lee
Aug 11, 2017·ACS Applied Materials & Interfaces·Ryan J GasvodaSumit Agarwal

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Citations

Mar 18, 2021·Langmuir : the ACS Journal of Surfaces and Colloids·Ryan J GasvodaSumit Agarwal
Nov 30, 2018·ACS Applied Materials & Interfaces·Harrison Sejoon KimJiyoung Kim
Oct 31, 2018·Langmuir : the ACS Journal of Surfaces and Colloids·Ryan J GasvodaSumit Agarwal

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