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Title: Same Precursor, Two Different Products: Comparing the Structural Evolution of In–Ga–O “Gel-Derived” Powders and Solution-Cast Films Using Pair Distribution Function Analysis

Abstract

Amorphous metal oxides are central to a variety of technological applications. In particular, indium gallium oxide has garnered attention as a thin-film transistor channel layer material. We examine the structural evolution of indium gallium oxide gel-derived powders and thin films using infrared vibrational spectroscopy, X-ray diffraction, and pair distribution function (PDF) analysis of X-ray total scattering from standard and normal incidence thin-film geometries (tfPDF). We find that the gel-derived powders and films from the same aqueous precursor evolve differently with temperature, forming mixtures of Ga-substituted In2O3 and In-substituted β-Ga2O3 with different degrees of substitution. X-ray total scattering and PDF analysis indicate that the majority phase for both the powders and films is an amorphous/nanocrystalline β-Ga2O3 phase, with a minor constituent of In2O3 with significantly larger coherence lengths. This amorphous β-Ga2O3 phase could not be identified using the conventional Bragg diffraction techniques traditionally used to study crystalline metal oxide thin films. The combination of Bragg diffraction and tfPDF provides a much more complete description of film composition and structure, which can be used to detail the effect of processing conditions and structure–property relationships. This study also demonstrates how structural features of amorphous materials, traditionally difficult to characterize by standard diffraction, canmore » be elucidated using tfPDF.« less

Authors:
ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [1]
  1. Univ. of Oregon, Eugene, OR (United States). Dept. of Chemistry and Biochemistry. Material Science Inst.
  2. Univ. of Copenhagen (Denmark). Dept. of Chemistry
Publication Date:
Research Org.:
Univ. of Oregon, Eugene, OR (United States); Univ. of Copenhagen (Denmark)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Danish Research Council (Denmark)
OSTI Identifier:
1418573
Grant/Contract Number:  
AC02-06CH11357; CHE-1606982
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 15; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Wood, Suzannah R., Woods, Keenan N., Plassmeyer, Paul N., Marsh, David A., Johnson, Darren W., Page, Catherine J., Jensen, Kirsten M. Ø., and Johnson, David C. Same Precursor, Two Different Products: Comparing the Structural Evolution of In–Ga–O “Gel-Derived” Powders and Solution-Cast Films Using Pair Distribution Function Analysis. United States: N. p., 2017. Web. doi:10.1021/jacs.7b02097.
Wood, Suzannah R., Woods, Keenan N., Plassmeyer, Paul N., Marsh, David A., Johnson, Darren W., Page, Catherine J., Jensen, Kirsten M. Ø., & Johnson, David C. Same Precursor, Two Different Products: Comparing the Structural Evolution of In–Ga–O “Gel-Derived” Powders and Solution-Cast Films Using Pair Distribution Function Analysis. United States. https://doi.org/10.1021/jacs.7b02097
Wood, Suzannah R., Woods, Keenan N., Plassmeyer, Paul N., Marsh, David A., Johnson, Darren W., Page, Catherine J., Jensen, Kirsten M. Ø., and Johnson, David C. Wed . "Same Precursor, Two Different Products: Comparing the Structural Evolution of In–Ga–O “Gel-Derived” Powders and Solution-Cast Films Using Pair Distribution Function Analysis". United States. https://doi.org/10.1021/jacs.7b02097. https://www.osti.gov/servlets/purl/1418573.
@article{osti_1418573,
title = {Same Precursor, Two Different Products: Comparing the Structural Evolution of In–Ga–O “Gel-Derived” Powders and Solution-Cast Films Using Pair Distribution Function Analysis},
author = {Wood, Suzannah R. and Woods, Keenan N. and Plassmeyer, Paul N. and Marsh, David A. and Johnson, Darren W. and Page, Catherine J. and Jensen, Kirsten M. Ø. and Johnson, David C.},
abstractNote = {Amorphous metal oxides are central to a variety of technological applications. In particular, indium gallium oxide has garnered attention as a thin-film transistor channel layer material. We examine the structural evolution of indium gallium oxide gel-derived powders and thin films using infrared vibrational spectroscopy, X-ray diffraction, and pair distribution function (PDF) analysis of X-ray total scattering from standard and normal incidence thin-film geometries (tfPDF). We find that the gel-derived powders and films from the same aqueous precursor evolve differently with temperature, forming mixtures of Ga-substituted In2O3 and In-substituted β-Ga2O3 with different degrees of substitution. X-ray total scattering and PDF analysis indicate that the majority phase for both the powders and films is an amorphous/nanocrystalline β-Ga2O3 phase, with a minor constituent of In2O3 with significantly larger coherence lengths. This amorphous β-Ga2O3 phase could not be identified using the conventional Bragg diffraction techniques traditionally used to study crystalline metal oxide thin films. The combination of Bragg diffraction and tfPDF provides a much more complete description of film composition and structure, which can be used to detail the effect of processing conditions and structure–property relationships. This study also demonstrates how structural features of amorphous materials, traditionally difficult to characterize by standard diffraction, can be elucidated using tfPDF.},
doi = {10.1021/jacs.7b02097},
journal = {Journal of the American Chemical Society},
number = 15,
volume = 139,
place = {United States},
year = {2017},
month = {3}
}

Journal Article:
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Cited by: 9 works
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Figures / Tables:

Figure 1 Figure 1: (a) FTIR spectra of indium gallium oxide films and (b) ATR-IR of indium gallium oxide gel powders annealed to various temperatures. The large absorption and shoulder feature, labeled “SiO”, around 1025 cm-1 is from thermal growth of SiO2 at the substrate/IGO interface at elevated temperatures.

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