First-principles studies of the structural and electronic properties of the (Ga1-xZnx)(N1-xOx) solid solution photocatalyst

Lin Lin Jensen, James Muckerman, Marshall D. Newton

Research output: Contribution to journalArticle

95 Citations (Scopus)

Abstract

Design of visible-light-driven photocatalytic materials has attracted intense interest in recent years in an attempt to enhance photonic efficiencies of hydrogen production via water splitting. Recent studies have shown that a solid solution of GaN and ZnO, (Ga1-xZnx)(N 1-xOx), can oxidize water under visible light in the presence of a sacrificial electron acceptor. Here we present a systematic study of the structural and electronic properties of this (Ga1-xZn x)(N1-xOx) solid solution as a function of zinc (oxygen) concentration, x, using density-functional theory (DFT). The DFT+ U approach has been adopted, and two different periodic supercells, the 16-atom (Ga8-nZnn)(N8-nOn) and 32-atom (Ga16-nZnn)(N16-nOn), have been used to model this solid solution. Results obtained from both supercells are in qualitative agreement with available experimental findings (in the lower concentration range x <0.25), although overall the larger 32-atom supercell provides a better description of the (Ga1-xZnx)(N 1-xOx) solid solution. Downward bowing of the band gap over the entire composition range has been observed for both supercells, and the minimum "experimental" band gap is estimated to be about 2.29 eV for the intermediate concentration x = 0.525. This suggests that the photocatalytic activity of this solid solution can be improved further by increasing its zinc (oxygen) concentration.

Original languageEnglish
Pages (from-to)3439-3446
Number of pages8
JournalJournal of Physical Chemistry C
Volume112
Issue number9
DOIs
Publication statusPublished - Mar 6 2008

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Photocatalysts
Electronic properties
Structural properties
Solid solutions
solid solutions
electronics
Atoms
Density functional theory
Zinc
Energy gap
zinc
Oxygen
density functional theory
atoms
Bending (forming)
water splitting
Water
hydrogen production
oxygen
Hydrogen production

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Electronic, Optical and Magnetic Materials
  • Surfaces, Coatings and Films
  • Energy(all)

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First-principles studies of the structural and electronic properties of the (Ga1-xZnx)(N1-xOx) solid solution photocatalyst. / Jensen, Lin Lin; Muckerman, James; Newton, Marshall D.

In: Journal of Physical Chemistry C, Vol. 112, No. 9, 06.03.2008, p. 3439-3446.

Research output: Contribution to journalArticle

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