Control of the Electrical Properties in Spinel Oxides by Manipulating the Cation Disorder

Paul F. Ndione, Yezhou Shi, Vladan Stevanovic, Stephan Lany, Andriy Zakutayev, Philip A. Parilla, John D. Perkins, Joseph J. Berry, David S. Ginley, Michael F. Toney

Research output: Contribution to journalArticlepeer-review

108 Scopus Citations

Abstract

In this work, the impact of cation disorder on the electrical properties of biaxially textured Co2ZnO4 and Co2NiO 4 thin films grown by pulsed laser deposition are investigated using a combination of experiment and theory. Resonant elastic X-ray diffraction along with conductivity measurements both before and after post-deposition annealing show that Co2ZnO4 and Co2NiO4 exhibit opposite changes of the conductivity with cation disorder, which can be traced back to their different ground-state atomic structures, being normal and inverse spinel, respectively. Electronic structure calculations identify a self-doping mechanism as the origin of conductivity. A novel thermodynamic model describes the non-equilibrium cation disorder in terms of an effective temperature. This work offers a way of controlling the conductivity in spinels in a quantitative manner by controlling the cation disorder and a new design principle whereby non-equilibrium growth can be used to create beneficial disorder. A combination of experiment and theory quantifies the dependence of the conductivity in Co2ZnO4 and Co2NiO 4 on the cation disorder. A self-doping mechanism is identified as the origin of conductivity and a thermodynamic model is used to describe the non-equilibrium cation disorder in terms of an effective temperature. The conductivity in spinels can be controlled by manipulating the cation disorder.

Original languageAmerican English
Pages (from-to)610-618
Number of pages9
JournalAdvanced Functional Materials
Volume24
Issue number5
DOIs
StatePublished - 2014

NREL Publication Number

  • NREL/JA-5900-62045

Keywords

  • annealing
  • cation disorder
  • conductivity
  • nickel cobalt oxides
  • spinels
  • zinc cobalt oxides

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