4.5 Article

The presence of superoxide ions and related dioxygen species in zinc oxide-A structural characterization by in situ Raman spectroscopy

Journal

JOURNAL OF RAMAN SPECTROSCOPY
Volume 53, Issue 12, Pages 2137-2146

Publisher

WILEY
DOI: 10.1002/jrs.6441

Keywords

Raman spectroscopy; solid-state-structures; superoxide ion; thin films; zinc oxide

Categories

Funding

  1. Ministry of Education, Science, and Technological Development of Serbia [1702201]
  2. Projekt DEAL

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Yellow-gray ZnO films are synthesized at room temperature by femtosecond pulsed laser deposition. In situ Raman investigations reveal the existence of superoxide ions, O-2(-), in these films, which are responsible for the yellow color.
Zinc oxide exhibits unique properties that are reflected in a wide variety of applications, particularly in the field of transparent, conductive films. However, less attention has been paid to their color. Here, we present the synthesis of yellow-gray ZnO films at room temperature by femtosecond pulsed laser deposition. In situ Raman investigations of these polycrystalline ZnO films reveal the existence of superoxide ions, O-2(-), in zinc oxide, which are responsible for the yellow color, and are also detected in ZnO powder and single crystals. In addition, further dioxygen species are identified in the samples, including the O-2-molecule. The negative charge excess caused by the dioxygen species creates metallic zinc as a byproduct. Structural analysis reveals an unforced realization of the dioxygen species in the ZnO lattice. Density functional theory (DFT) calculations support the assumed structural displacements as well as the observed, unexpected Raman bands. These results open up completely new insights into the behavior of ZnO.

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