期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 144, 期 26, 页码 11757-11766出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c03752
关键词
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资金
- Department of Energy [DE-SC0004782]
- National Research Foundation (NRF) - Ministry of Science and ICT, Korea [NRF-2021R1A4A1033155]
- ANID FONDECYT [11180906]
- Research Training Group 1782 - Deutsche Forschungsgemeinschaft (DFG)
- NEW LIMITS, a center in nCORE, a Semiconductor Research Corporation (SRC) program - NIST [70NANB17H041]
This study systematically investigates the growth characteristics of aluminum oxide films in atomic layer deposition (ALD) processes. The results show that the precursor structure plays a crucial role in both chemical reactivity and geometrical constraints during deposition.
The adsorption of metalorganic and metal halide precursors on the SiO2 surface plays an essential role in thin-film deposition processes such as atomic layer deposition (ALD). In the case of aluminum oxide (Al2O3) films, the growth characteristics are influenced by the precursor structure, which controls both chemical reactivity and the geometrical constraints during deposition. In this work, a systematic study using a series of Al(CH3)(x)Cl3-x (x = 0, 1, 2, and 3) and Al(CyH2y+1) 3 (y = 1, 2, and 3) precursors is carried out using a combination of experimental spectroscopic techniques together with density functional theory calculations and Monte Carlo simulations to analyze differences across precursor molecules. Results show that reactivity and steric hindrance mutually influence the ALD surface reaction. The increase in the number of chlorine ligands in the precursor shifts the deposition temperature higher, an effect attributed to more favorable binding of the intermediate species due to higher Lewis acidity, while differences between precursors in film growth per cycle are shown to originate from variations in adsorption activation barriers and size-dependent saturation coverage. Comparison between the theoretical and experimental results indicates that the Al(CyH2y+1)(3) precursors are favored to undergo two ligand exchange reactions upon adsorption at the surface, whereas only a single Cl-ligand exchange reaction is energetically favorable upon adsorption by the AlCl3 precursor. By pursuing the first-principles design of ALD precursors combined with experimental analysis of thin-film growth, this work enables a robust understanding of the effect of precursor chemistry on ALD processes.
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