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Pyridine-Catalyzed Atomic Layer Deposition of SiO2 from Hexachlorodisilane and Water: An In Situ Mechanistic Study

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CHEMISTRY OF MATERIALS
卷 35, 期 10, 页码 4100-4108

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AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.3c00621

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Pyridine-catalyzed atomic layer deposition (ALD) of SiO2 from hexachlorodisilane and water was studied. Self-limiting growth of SiO2 by catalytic ALD has been achieved when both half-reactions are catalyzed by pyridine. The unexpected growth of SiO2, when only one half-reaction was catalyzed, was caused by the presence of residual pyridine that had not yet desorbed from the previous half-reaction. The retardation of catalyst desorption was more prominent on the OH-terminated SiO2 surface than on the Cl-terminated surface, which is related to the significantly higher desorption energy of pyridine species on the hydroxyl surface calculated using density functional theory.
Pyridine-catalyzed atomic layer deposition (ALD) of SiO2 from hexachlorodisilane and water was studied by in situ analyses using Fourier-transform infrared spectrometry and a quartz crystal microbalance. Although it has been observed that ALD SiO2 can grow even when only one half-reaction is catalyzed, typical self-limiting growth of SiO2 by catalytic ALD has been achieved when both half-reactions are catalyzed by pyridine. The in situ analyses revealed that the unexpected growth of SiO2, when only one half-reaction was catalyzed, was caused by the presence of residual pyridine that had not yet desorbed from the previous half-reaction. The retardation of catalyst desorption was more prominent on the OH-terminated SiO2 surface than on the Cl-terminated surface, which is related to the significantly higher desorption energy of pyridine species on the hydroxyl surface calculated using density functional theory.

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