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

doi:10.1021/jacs.7b02097

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 In ₂O ₃ and In-substituted β-Ga ₂O ₃ 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-Ga ₂O ₃ phase, with a minor constituent of In ₂O ₃ with significantly larger coherence lengths. This amorphous β-Ga ₂O ₃ 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 ofmore »« less

Authors:

^[1]; Woods, Keenan N. ^[1]; Plassmeyer, Paul N. ^[1]; Marsh, David A. ^[1];

^[1];

^[1]; Jensen, Kirsten M. Ø. ^[2];

^[1]

Univ. of Oregon, Eugene, OR (United States). Dept. of Chemistry and Biochemistry. Material Science Inst.
Univ. of Copenhagen (Denmark). Dept. of Chemistry

Publication Date:: 2017-03-22

Research Org.:: Univ. of Oregon, Eugene, OR (United States); Univ. of Copenhagen (Denmark)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); 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.

Copy to clipboard


                    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.  doi:10.1021/jacs.7b02097.

Copy to clipboard


                    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.  doi:10.1021/jacs.7b02097.  https://www.osti.gov/servlets/purl/1418573.

Copy to clipboard


                    
@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}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (DOE)

Publisher's Version of Record

DOI: 10.1021/jacs.7b02097

Other availability

Search WorldCat to find libraries that may hold this journal

Citation Metrics:

Cited by: 7 works

Citation information provided by
Web of Science

Figures / Tables:

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.

All figures and tables (8 total)

Save / Share:

Export Metadata

Save to My Library

Works referencing / citing this record:

Local atomic structure of thin and ultrathin films via rapid high-energy X-ray total scattering at grazing incidence
journal, February 2019

Dippel, Ann-Christin; Roelsgaard, Martin; Boettger, Ulrich
IUCrJ, Vol. 6, Issue 2
DOI: 10.1107/s2052252519000514

Figures / Tables found in this record:

Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.

Similar records in OSTI.GOV collections:

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 Wood, Suzannah R. ; Woods, Keenan N. ; Plassmeyer, Paul N. ; ... - Journal of the American Chemical Society

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. In this work 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 scatteringmore »« less
DOI: 10.1021/jacs.7b02097
Effect of postdeposition annealing on the electrical properties of β-Ga{sub 2}O{sub 3} thin films grown on p-Si by plasma-enhanced atomic layer deposition

Journal Article Altuntas, Halit, E-mail: altunhalit@gmail.com ; Donmez, Inci ; Ozgit-Akgun, Cagla ; ... - Journal of Vacuum Science and Technology. A, Vacuum, Surfaces and Films

Ga{sub 2}O{sub 3} dielectric thin films were deposited on (111)-oriented p-type silicon wafers by plasma-enhanced atomic layer deposition using trimethylgallium and oxygen plasma. Structural analysis of the Ga{sub 2}O{sub 3} thin films was carried out using grazing-incidence x-ray diffraction. As-deposited films were amorphous. Upon postdeposition annealing at 700, 800, and 900 °C for 30 min under N{sub 2} ambient, films crystallized into β-form monoclinic structure. Electrical properties of the β-Ga{sub 2}O{sub 3} thin films were then investigated by fabricating and characterizing Al/β-Ga{sub 2}O{sub 3}/p-Si metal–oxide-semiconductor capacitors. The effect of postdeposition annealing on the leakage current densities, leakage current conduction mechanisms, dielectric constants,more »« less
DOI: 10.1116/1.4875935
Gallium Oxide Nanostructures for High Temperature Sensors

Technical Report Chintalapalle, Ramana V.

Gallium oxide (Ga ₂O ₃) thin films were produced by sputter deposition by varying the substrate temperature (T _s) in a wide range (T _s=25-800 °C). The structural characteristics and electronic properties of Ga ₂O ₃ films were evaluated using X-ray diffraction (XRD), scanning electron microscopy (SEM), energy-dispersive X-ray spectrometry (EDS), Rutherford backscattering spectrometry (RBS) and spectrophotometric measurements. The effect of growth temperature is significant on the chemistry, crystal structure and morphology of Ga ₂O ₃ films. XRD and SEM analyses indicate that the Ga ₂O ₃ films grown at lower temperatures were amorphous while those grown at T _s≥500more »« less
DOI: 10.2172/1261782

Full Text Available
Alkoxide routes to Inorganic Materials

Thesis/Dissertation Thomas, George Harrison

An all alkoxide solution chemistry utilizing metal 2-methoxyethoxide complexes in 2-methoxyethanol was used to deposit thin-films of metal oxides on single-crystal metal oxide substrates and on biaxially textured metal substrates. This same chemistry was used to synthesize complex metal oxide nanoparticles. Nuclear Magnetic Resonance spectroscopy was used to study precursor solutions of the alkaline niobates and tantalates. Film crystallization temperatures were determined from x-ray diffraction patterns of powders derived from the metal oxide precursor solutions. Film structure was determined via x-ray diffraction. Film morphology was studied using scanning electron microscopy (SEM) and atomic force microscopy (AFM). Epitaxial thin-films of strontiummore »« less
DOI: 10.2172/971209

Full Text Available
Chemical bonding, optical constants, and electrical resistivity of sputter-deposited gallium oxide thin films

Journal Article Ramana, C. V., E-mail: rvchintalapalle@utep.edu ; Rubio, E. J. ; Barraza, C. D. ; ... - Journal of Applied Physics

Gallium oxide (Ga{sub 2}O{sub 3}) thin films were made by sputter deposition employing a Ga{sub 2}O{sub 3} ceramic target for sputtering. The depositions were made over a wide range of substrate temperatures (T{sub s}), from 25 to 600 °C. The effect of T{sub s} on the chemical bonding, surface morphological characteristics, optical constants, and electrical properties of the grown films was evaluated using X-ray photoelectron spectroscopy (XPS), atomic force microscopy (AFM), spectroscopic ellipsometry (SE), and four-point probe measurements. XPS analyses indicate the binding energies (BE) of the Ga 2p doublet, i.e., the Ga 2p{sub 3/2} and Ga 2p{sub 1/2} peaks, aremore »« less
DOI: 10.1063/1.4862186

Similar Records

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

Citation Formats

Figures / Tables:

Local atomic structure of thin and ultrathin films via rapid high-energy X-ray total scattering at grazing incidence journal, February 2019

Local atomic structure of thin and ultrathin films via rapid high-energy X-ray total scattering at grazing incidence
journal, February 2019