Article (Scientific journals)
Elucidating the growth mechanism of ZnO films by atomic layer deposition with oxygen gas via isotopic tracking
Nguyen, Tai; Valle, Nathalie; Guillot, Jerome et al.
2021In JOURNAL OF MATERIALS CHEMISTRY C, 9 (12), p. 4307-4315
Peer reviewed
 

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Abstract :
[en] The growth process of zinc oxide (ZnO) thin films by atomic layer deposition (ALD) accompanied by the presence of oxygen gas pulsing is investigated by means of the isotopic tracking of oxygen O-18 from the water precursor and oxygen O-16 from the gas. In a previous study [T. Nguyen et al., Results Mater., 2020, 6, 100088, DOI: 10.1016/j.rinma.2020.100088], by means of structural, electrical, and optical characterizations, we identified key growth parameters of this unusual ALD process. Unexpectedly, the influence of molecular oxygen on the crystallography, microstructure, and morphology of the hundred-nanometer- to micrometer-thick ZnO films was significant. In this study, we present an unprecedented methodology by combining isotopic tracers with mass spectrometry to elucidate the role of the two different sources of oxygen atoms during the evolution of the growth. Notably, the use of in situ quartz crystal microbalance (QCM) and Secondary Ion Mass Spectrometry (SIMS) reveals new insights into the reaction mechanism for ZnO thin film growth. On the one hand, the non-negative mass change during the ZnO growth without O-2 gas is attributed to the presence of bare zinc atoms on the surface due to the reaction between monoethyl zinc and hydroxyl groups of the water precursor after the diethyl zinc pulse. On the other hand, the detection of ZnxOyC2H5- ions by Time-of-Flight SIMS (TOF-SIMS) and the mass increase during the O-2 pulse suggest a new reaction mechanism for the ZnO thin film growth in the presence of gaseous O-2 where the ethyl ligand of the zinc precursor can react with O-2 to form ethylperoxy radicals. The formations of the ethylperoxy zinc and/or zinc atoms lead to more adsorption of water to form ethylhydroperoxide during the water pulse, inducing the positive mass change. The use of an isotopic substitution allowed us to unambiguously associate the mass gain with the gradual incorporation of gaseous oxygen throughout the growth process and thereby support the chemical reaction.
Disciplines :
Physics
Author, co-author :
Nguyen, Tai;  Luxembourg Institute of Science & Technology - LIST
Valle, Nathalie;  Luxembourg Institute of Science & Technology - LIST
Guillot, Jerome;  Luxembourg Institute of Science & Technology - LIST
Bour, Jerome;  Luxembourg Institute of Science & Technology - LIST
Adjeroud, Noureddine;  Luxembourg Institute of Science & Technology - LIST
Fleming, Yves ;  Luxembourg Institute of Science & Technology - LIST
Guennou, Mael  ;  University of Luxembourg > Faculty of Science, Technology and Medicine (FSTM) > Department of Physics and Materials Science (DPHYMS)
Jean-Nicolas, Audinot;  Luxembourg Institute of Science & Technology - LIST
El Adib, Brahime;  Luxembourg Institute of Science & Technology - LIST
Joly, Raoul;  Luxembourg Institute of Science & Technology - LIST
Arl, Didier;  Luxembourg Institute of Science & Technology - LIST
Frache, Gilles;  Luxembourg Institute of Science & Technology - LIST
Polesel-Maris, Jerome;  Luxembourg Institute of Science & Technology - LIST
More authors (3 more) Less
External co-authors :
no
Title :
Elucidating the growth mechanism of ZnO films by atomic layer deposition with oxygen gas via isotopic tracking
Publication date :
2021
Journal title :
JOURNAL OF MATERIALS CHEMISTRY C
ISSN :
2050-7526
Publisher :
ROYAL SOC CHEMISTRY, THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS ENGLAND, Unknown/unspecified
Volume :
9
Issue :
12
Pages :
4307-4315
Peer reviewed :
Peer reviewed
FnR Project :
FNR10935404 - Materials For Sensing And Energy Harvesting, 2015 (01/10/2016-31/03/2023) - Emmanuel Defay
Commentary :
Article
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since 12 December 2021

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