Using design principles to systematically plan the synthesis of hole-conducting transparent oxides: Cu3VO4 and Ag 3VO4 as a case study

Giancarlo Trimarchi, Haowei Peng, Jino Im, Arthur J Freeman, Veerle Cloet, Adam Raw, Kenneth R Poeppelmeier, Koushik Biswas, Stephan Lany, Alex Zunger

Research output: Contribution to journalArticle

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Abstract

In order to address the growing need for p-type transparent conducting oxides (TCOs), we present a materials design approach that allows to search for materials with desired properties. We put forward a set of design principles (DPs) that a material must meet in order to qualify as a p-type TCO. We then start from two prototype p-type binary oxides, i.e., Cu2O and Ag 2O, and define a large group of compounds in which to search for unique candidate materials. From this set of compounds, we extracted two oxovanadates, Cu3VO4 and Ag3VO4, which serve as a case study to show the application of the proposed materials selection procedure driven by the DPs. Polycrystalline Ag3VO 4 was synthesized by a water-based hydrothermal technique, whereas Cu3VO4 was prepared by a solid-state reaction. The theoretical study of the thermochemistry, based on first-principles electronic structure methods, demonstrates that Cu3VO4 and α-Ag3VO4 are p-type materials that show intrinsic hole-producing defects along with a low concentration of "hole- killing" defects. Owing to its near-perfect stoichiometry, Ag 3VO4 has a rather low hole concentration, which coincides with the experimentally determined conductivity limit of 0.002 S/cm. In contrast, Cu3VO4 is highly off stoichiometric, Cu 3-xVO4 (x=0.15), which raises the amount of holes, but due to its black color, it does not fulfill the requirements for a p-type TCO. The onset of optical absorption in α-Ag3VO4 is calculated to be 2.6 eV, compared to the experimentally determined value of 2.1 eV, which brings it to the verge of transparency.

Original languageEnglish
Article number165116
JournalPhysical Review B - Condensed Matter and Materials Physics
Volume84
Issue number16
DOIs
Publication statusPublished - Oct 14 2011

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Oxides
conduction
oxides
synthesis
materials selection
thermochemistry
defects
Thermochemistry
Hole concentration
Defects
low concentrations
stoichiometry
optical absorption
Solid state reactions
Stoichiometry
Transparency
Light absorption
prototypes
Electronic structure
electronic structure

ASJC Scopus subject areas

  • Condensed Matter Physics
  • Electronic, Optical and Magnetic Materials

Cite this

Using design principles to systematically plan the synthesis of hole-conducting transparent oxides : Cu3VO4 and Ag 3VO4 as a case study. / Trimarchi, Giancarlo; Peng, Haowei; Im, Jino; Freeman, Arthur J; Cloet, Veerle; Raw, Adam; Poeppelmeier, Kenneth R; Biswas, Koushik; Lany, Stephan; Zunger, Alex.

In: Physical Review B - Condensed Matter and Materials Physics, Vol. 84, No. 16, 165116, 14.10.2011.

Research output: Contribution to journalArticle

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