skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

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

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/jacs.7b02097· OSTI ID:1418573

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.

Research Organization:
Univ. of Oregon, Eugene, OR (United States); Univ. of Copenhagen (Denmark)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Danish Research Council (Denmark)
Grant/Contract Number:
AC02-06CH11357; CHE-1606982
OSTI ID:
1418573
Journal Information:
Journal of the American Chemical Society, Vol. 139, Issue 15; ISSN 0002-7863
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 11 works
Citation information provided by
Web of Science

References (49)

Engineering of band gap states of amorphous SiZnSnO semiconductor as a function of Si doping concentration journal November 2016
Probing the highly transparent and conducting SnO x /Au/SnO x structure for futuristic TCO applications journal January 2016
Interfacial control of oxygen vacancy doping and electrical conduction in thin film oxide heterostructures journal June 2016
Transparent ferromagnetic and semiconducting behavior in Fe-Dy-Tb based amorphous oxide films journal June 2016
Metal oxides for optoelectronic applications journal March 2016
Spray-combustion synthesis: Efficient solution route to high-performance oxide transistors journal March 2015
Linear topology in amorphous metal oxide electrochromic networks obtained via low-temperature solution processing journal August 2016
Measurement and Modeling of Short and Medium Range Order in Amorphous Ta2O5 Thin Films journal August 2016
Solution-processed inorganic semiconductors journal January 2004
Oxide Semiconductor Thin-Film Transistors: A Review of Recent Advances journal May 2012
Amorphous Oxide Semiconductors for High-Performance Flexible Thin-Film Transistors journal May 2006
Ionic amorphous oxide semiconductors: Material design, carrier transport, and device application journal June 2006
Disorder and instability processes in amorphous conducting oxides journal June 2008
Recurring polyhedral motifs in the amorphous indium gallium zinc oxide network: Polyhedral motifs in indium gallium zinc oxide network journal February 2017
Room-temperature fabrication of transparent flexible thin-film transistors using amorphous oxide semiconductors journal November 2004
Role of order and disorder on the electronic performances of oxide semiconductor thin film transistors journal February 2007
Nanostructure of sol–gel films by x-ray specular reflectivity journal January 2002
Density-modulated alumina-based nanometre films prepared by sol–gel technique journal July 2005
Functional Ultrathin Films and Nanolaminates from Aqueous Solutions journal January 2013
Multilayer model for determining the thickness and refractive index of sol–gel coatings via laser ellipsometry journal March 2013
Amorphous In–Ga–Zn Oxide Semiconducting Thin Films with High Mobility from Electrochemically Generated Aqueous Nanocluster Inks journal August 2015
Electron diffraction analysis of polycrystalline and amorphous thin films journal November 1988
Non-uniform Composition Profiles in Inorganic Thin Films from Aqueous Solutions journal December 2015
Application of HAADF STEM image analysis to structure determination in rotationally disordered and amorphous multilayered films journal June 2016
New Technique for Investigating Noncrystalline Structures: Fourier Analysis of the Extended X-Ray—Absorption Fine Structure journal November 1971
Application of Differential Anomalous X-Ray Scattering to Structural Studies of Amorphous Materials journal June 1981
Structure and Disorder in Amorphous Alumina Thin Films: Insights from High-Resolution Solid-State NMR journal July 2010
Probing of 2 dimensional confinement-induced structural transitions in amorphous oxide thin film journal February 2014
Structure and bonding in photodiffused amorphous Ag- GeSe 2 thin films journal December 1988
The structural characterization of amorphous thin films and coatings in their as-deposited state using x-rays at shallow angles of incidence journal January 1997
Demonstration of thin film pair distribution function analysis (tfPDF) for the study of local structure in amorphous and crystalline thin films journal July 2015
The atomic level journey from aqueous polyoxometalate to metal oxide journal January 2015
Amorphous Mixed-Metal Oxide Thin Films from Aqueous Solution Precursors with Near-Atomic Smoothness journal December 2016
Scalability and homogeneity of slot die-coated metal oxide semiconductor for TFTs: Scalability and homogeneity of coated metal oxide journal May 2016
Solution-processable metal oxide semiconductors for thin-film transistor applications journal January 2013
Low-temperature fabrication of high-performance metal oxide thin-film electronics via combustion processing journal April 2011
Low-Temperature Solution-Processed Amorphous Indium Tin Oxide Field-Effect Transistors journal August 2009
WinPLOTR: A Windows Tool for Powder Diffraction Pattern Analysis journal October 2001
Rapid-acquisition pair distribution function (RA-PDF) analysis journal November 2003
PDFfit2 and PDFgui: computer programs for studying nanostructure in crystals journal July 2007
Aqueous Solution-Deposited Gallium Oxide Dielectric for Low-Temperature, Low-Operating-Voltage Indium Oxide Thin-Film Transistors: A Facile Route to Green Oxide Electronics journal June 2015
Hexaaqua Metal Complexes for Low-Temperature Formation of Fully Metal Oxide Thin-Film Transistors journal August 2015
Gallium(iii) hydration in aqueous solution of perchlorate, nitrate and sulfate. Raman and 71-Ga NMR spectroscopic studies and ab initio molecular orbital calculations of gallium(iii) water clustersElectronic supplementary information (ESI) available: Unscaled HF/6-31+G* frequencies, intensities and force constants of the hexaaqua-Ga(iii) ion, octadeca-aqua gallium(iii) and octadeca-aqua gallium(iii) cluster. See http://www.rsc.org/suppdata/cp/b2/b202567c/ journal August 2002
Indium( iii ) hydration in aqueous solutions of perchlorate, nitrate and sulfate. Raman and infrared spectroscopic studies and ab-initio molecular orbital calculations of indium( iii )–water clusters journal January 2004
Low-temperature growth of silicon dioxide films: A study of chemical bonding by ellipsometry and infrared spectroscopy journal March 1987
Synthesis and Solid-State Structural Characterization of a Series of Aqueous Heterometallic Tridecameric Group 13 Clusters journal March 2015
Phase Equilibria in the Ga2O3In2O3 System journal January 1997
Investigations in the β-Ga2O3/In2O3 system: crystal growth of solid solutions journal November 2000
Tunable growth of (GaxIn1−x)2O3 nanowires by water vapor journal July 2012

Cited By (4)

Time-resolved grazing-incidence pair distribution functions during deposition by radio-frequency magnetron sputtering text January 2019
Local atomic structure of thin and ultrathin films via rapid high-energy X-ray total scattering at grazing incidence journal February 2019
Time-resolved grazing-incidence pair distribution functions during deposition by radio-frequency magnetron sputtering text January 2019
Local atomic structure of thin and ultrathin films via rapid high-energy X-ray total scattering at grazing incidence text January 2019

Figures / Tables (8)