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Title: Site Dependency of the High Conductivity of Ga 2 In 6 Sn 2 O 16 : The Role of the 7-Coordinate Site

Abstract

In 6-coordinated cation sites, we find that it is the fundamental building block of the most effective transparent conducting oxides. Ga 2In 6SnO 16, however, maintains 4-, 6-, 7-, and 8-coordinated cation sites and still exhibits desirable transparency and high conductivity. To investigate the potential impact of these alternative sites, we partially replace the Sn in Ga 2In 6Sn 2O 16 with Ti, Zr, or Hf and use a combined approach of density functional theory-based calculations, X-ray diffraction, and neutron diffraction to establish that the substitution occurs preferentially on the 7-coordinate site. Conversely to Sn, the empty d orbitals of Ti, Zr, and Hf promote spd covalency with the surrounding oxygen, which decreases the conductivity. Pairing the substitutional site preference with the magnitude of this decrease demonstrates that the 7-coordinate site is the V major contributor to conductivity. The optical band gaps, in contrast, are shown to be site-independent and composition-dependent. After all 7-coordinate Sn has been replaced, the continued substitution of Sn results in the formation of a 7-coordinate In antisite or replacement of 6-coordinate Sn, depending on the identity of the d(0) substitute.

Authors:
 [1];  [2];  [3];  [1];  [1];  [1]
  1. Northwestern Univ., Evanston, IL (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1261489
Grant/Contract Number:  
AC05-00OR22725; DGE-1324585; FG02-08ER46536
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 27; Journal Issue: 23; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Rickert, Karl, Huq, Ashfia, Lapidus, Saul H., Wustrow, Allison, Ellis, Donald E., and Poeppelmeier, Kenneth R. Site Dependency of the High Conductivity of Ga 2 In 6 Sn 2 O 16 : The Role of the 7-Coordinate Site. United States: N. p., 2015. Web. doi:10.1021/acs.chemmater.5b03790.
Rickert, Karl, Huq, Ashfia, Lapidus, Saul H., Wustrow, Allison, Ellis, Donald E., & Poeppelmeier, Kenneth R. Site Dependency of the High Conductivity of Ga 2 In 6 Sn 2 O 16 : The Role of the 7-Coordinate Site. United States. doi:10.1021/acs.chemmater.5b03790.
Rickert, Karl, Huq, Ashfia, Lapidus, Saul H., Wustrow, Allison, Ellis, Donald E., and Poeppelmeier, Kenneth R. Wed . "Site Dependency of the High Conductivity of Ga 2 In 6 Sn 2 O 16 : The Role of the 7-Coordinate Site". United States. doi:10.1021/acs.chemmater.5b03790. https://www.osti.gov/servlets/purl/1261489.
@article{osti_1261489,
title = {Site Dependency of the High Conductivity of Ga 2 In 6 Sn 2 O 16 : The Role of the 7-Coordinate Site},
author = {Rickert, Karl and Huq, Ashfia and Lapidus, Saul H. and Wustrow, Allison and Ellis, Donald E. and Poeppelmeier, Kenneth R.},
abstractNote = {In 6-coordinated cation sites, we find that it is the fundamental building block of the most effective transparent conducting oxides. Ga2In6SnO16, however, maintains 4-, 6-, 7-, and 8-coordinated cation sites and still exhibits desirable transparency and high conductivity. To investigate the potential impact of these alternative sites, we partially replace the Sn in Ga2In6Sn2O16 with Ti, Zr, or Hf and use a combined approach of density functional theory-based calculations, X-ray diffraction, and neutron diffraction to establish that the substitution occurs preferentially on the 7-coordinate site. Conversely to Sn, the empty d orbitals of Ti, Zr, and Hf promote spd covalency with the surrounding oxygen, which decreases the conductivity. Pairing the substitutional site preference with the magnitude of this decrease demonstrates that the 7-coordinate site is the V major contributor to conductivity. The optical band gaps, in contrast, are shown to be site-independent and composition-dependent. After all 7-coordinate Sn has been replaced, the continued substitution of Sn results in the formation of a 7-coordinate In antisite or replacement of 6-coordinate Sn, depending on the identity of the d(0) substitute.},
doi = {10.1021/acs.chemmater.5b03790},
journal = {Chemistry of Materials},
number = 23,
volume = 27,
place = {United States},
year = {2015},
month = {11}
}

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