Investigating the Relative Stabilities and Electronic Properties of Small Zinc Oxide Clusters


GUNARATNE K. D. D., Berkdemir C., HARMON C. L., CASTLEMAN A. W.

JOURNAL OF PHYSICAL CHEMISTRY A, cilt.116, sa.51, ss.12429-12437, 2012 (SCI-Expanded) identifier

  • Yayın Türü: Makale / Tam Makale
  • Cilt numarası: 116 Sayı: 51
  • Basım Tarihi: 2012
  • Doi Numarası: 10.1021/jp3029374
  • Dergi Adı: JOURNAL OF PHYSICAL CHEMISTRY A
  • Derginin Tarandığı İndeksler: Science Citation Index Expanded (SCI-EXPANDED), Scopus
  • Sayfa Sayıları: ss.12429-12437
  • Erciyes Üniversitesi Adresli: Hayır

Özet

We report a combined experimental and theoretical study investigating small zinc oxide clusters. A laser vaporization source and a time-of-flight (TOF) mass spectrometer are employed to produce and identify anionic clusters in the ZnnOm (n = 1-6, m = 1-7) size regime. The adiabatic detachment energy (ADE) and vertical detachment energy (VDE) of Zn3O3- and Zn3O4- clusters are determined via anion photoelectron spectroscopy. We have utilized density functional theory (DFT) calculations to explore the possible geometries of neutral and anionic Zn3Om (m = 3-5) clusters, while the theoretical ADE and VDE values are compared with experimental results. The experimentally observed relative abundances among the Zn3Om- (m = 3-5) clusters are investigated through calculations of the detachment energies, dissociation energies, and HOMO-LUMO gaps. We find that the Zn3O3 cluster maintains enhanced stability compared to their oxygen-rich counterparts. Furthermore, by coupling the experimentally obtained photoelectron angular distributions of Zn3O3- and Zn3O4- with electronic structure calculations, the nature of the highest occupied molecular orbitals is discussed, with the goal of aiding the isolation (ligand-capped)/deposition of these building blocks.