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Title: An Atomistic View of the Incipient Growth of Zinc Oxide Nanolayers

Abstract

The growth of zinc oxide thin films by atomic layer deposition is believed to proceed through an embryonic step in which three-dimensional nanoislands form and then coalesce to trigger a layer-by-layer growth mode. This transient initial state is characterized by a poorly ordered atomic structure, which may be inaccessible by X-ray diffraction techniques. Here in this work, we apply X-ray absorption spectroscopy in situ to address the local structure of Zn after each atomic layer deposition cycle, using a custom-built reactor mounted at a synchrotron beamline, and we shed light on the atomistic mechanisms taking place during the first stages of the growth. We find that such mechanisms are surprisingly different for zinc oxide growth on amorphous (silica) and crystalline (sapphire) substrate. Ab initio simulations and quantitative data analysis allow the formulation of a comprehensive growth model, based on the different effects of surface atoms and grain boundaries in the nanoscale islands, and the consequent induced local disorder. From a comparison of these spectroscopy results with those from X-ray diffraction reported recently, we observe that the final structure of the zinc oxide nanolayers depends strongly on the mechanisms taking place during the initial stages of growth. Finally, the approach followedmore » here for the case of zinc oxide will be of general interest for characterizing and optimizing the growth and properties of more complex nanostructures.« less

Authors:
 [1];  [2];  [2];  [2];  [3];  [2];  [2];  [2];  [3];  [3];  [2];  [2];  [4];  [1]
  1. Source optimisee de lumiere d'energie intermediaire du LURE (SOLEIL),Gif-sur-Yvette (France). Beamline SIRIUS
  2. Univ. Grenoble Alpes (France)
  3. Aix-Marseille Univ., Marseille (France); Inst. Materiaux Microelectronique Nanosciences de Provence (IM2NP)
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1339135
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Crystal Growth and Design
Additional Journal Information:
Journal Volume: 16; Journal Issue: 9; Journal ID: ISSN 1528-7483
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Chu, Manh Hung, Tian, Liang, Chaker, Ahmad, Cantelli, Valentina, Ouled, Toufik, Boichot, Raphaël, Crisci, Alexandre, Lay, Sabine, Richard, Marie-Ingrid, Thomas, Olivier, Deschanvres, Jean-Luc, Renevier, Hubert, Fong, Dillon D., and Ciatto, Gianluca. An Atomistic View of the Incipient Growth of Zinc Oxide Nanolayers. United States: N. p., 2016. Web. doi:10.1021/acs.cgd.6b00844.
Chu, Manh Hung, Tian, Liang, Chaker, Ahmad, Cantelli, Valentina, Ouled, Toufik, Boichot, Raphaël, Crisci, Alexandre, Lay, Sabine, Richard, Marie-Ingrid, Thomas, Olivier, Deschanvres, Jean-Luc, Renevier, Hubert, Fong, Dillon D., & Ciatto, Gianluca. An Atomistic View of the Incipient Growth of Zinc Oxide Nanolayers. United States. doi:10.1021/acs.cgd.6b00844.
Chu, Manh Hung, Tian, Liang, Chaker, Ahmad, Cantelli, Valentina, Ouled, Toufik, Boichot, Raphaël, Crisci, Alexandre, Lay, Sabine, Richard, Marie-Ingrid, Thomas, Olivier, Deschanvres, Jean-Luc, Renevier, Hubert, Fong, Dillon D., and Ciatto, Gianluca. Tue . "An Atomistic View of the Incipient Growth of Zinc Oxide Nanolayers". United States. doi:10.1021/acs.cgd.6b00844. https://www.osti.gov/servlets/purl/1339135.
@article{osti_1339135,
title = {An Atomistic View of the Incipient Growth of Zinc Oxide Nanolayers},
author = {Chu, Manh Hung and Tian, Liang and Chaker, Ahmad and Cantelli, Valentina and Ouled, Toufik and Boichot, Raphaël and Crisci, Alexandre and Lay, Sabine and Richard, Marie-Ingrid and Thomas, Olivier and Deschanvres, Jean-Luc and Renevier, Hubert and Fong, Dillon D. and Ciatto, Gianluca},
abstractNote = {The growth of zinc oxide thin films by atomic layer deposition is believed to proceed through an embryonic step in which three-dimensional nanoislands form and then coalesce to trigger a layer-by-layer growth mode. This transient initial state is characterized by a poorly ordered atomic structure, which may be inaccessible by X-ray diffraction techniques. Here in this work, we apply X-ray absorption spectroscopy in situ to address the local structure of Zn after each atomic layer deposition cycle, using a custom-built reactor mounted at a synchrotron beamline, and we shed light on the atomistic mechanisms taking place during the first stages of the growth. We find that such mechanisms are surprisingly different for zinc oxide growth on amorphous (silica) and crystalline (sapphire) substrate. Ab initio simulations and quantitative data analysis allow the formulation of a comprehensive growth model, based on the different effects of surface atoms and grain boundaries in the nanoscale islands, and the consequent induced local disorder. From a comparison of these spectroscopy results with those from X-ray diffraction reported recently, we observe that the final structure of the zinc oxide nanolayers depends strongly on the mechanisms taking place during the initial stages of growth. Finally, the approach followed here for the case of zinc oxide will be of general interest for characterizing and optimizing the growth and properties of more complex nanostructures.},
doi = {10.1021/acs.cgd.6b00844},
journal = {Crystal Growth and Design},
number = 9,
volume = 16,
place = {United States},
year = {2016},
month = {8}
}

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