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

Journal Article · · Crystal Growth and Design
 [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

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.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1339135
Journal Information:
Crystal Growth and Design, Vol. 16, Issue 9; ISSN 1528-7483
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 11 works
Citation information provided by
Web of Science

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Cited By (4)

The initial stages of ZnO atomic layer deposition on atomically flat In 0.53 Ga 0.47 As substrates journal January 2018
Role of Co 2 C in ZnO-promoted Co Catalysts for Alcohol Synthesis from Syngas journal December 2018
In Situ Ellipsometry Study of the Early Stage of ZnO Atomic Layer Deposition on In 0.53 Ga 0.47 As journal January 2020
Evaluation of Alternative Atomistic Models for the Incipient Growth of ZnO by Atomic Layer Deposition journal March 2017

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