Document Type

Article

Original Publication Date

1998

Journal/Book/Conference Title

Journal of Chemical Physics

Volume

109

Issue

4

DOI of Original Publication

10.1063/1.476675

Comments

Originally published at http://dx.doi.org/10.1063/1.476675

Date of Submission

October 2015

Abstract

Using molecular orbital approach and the generalized gradient approximation in the density functional theory, we have calculated the equilibrium geometries, binding energies, ionization potentials, and vertical and adiabatic electron affinities of SinOm clusters (n⩽6,m⩽12). The calculations were carried out using both Gaussian and numerical form for the atomic basis functions. Both procedures yield very similar results. The bonding in SinOm clusters is characterized by a significant charge transfer between the Si and O atoms and is stronger than in conventional semiconductor clusters. The bond distances are much less sensitive to cluster size than seen for metallic clusters. Similarly, calculated energy gaps between the highest occupied and lowest unoccupied molecular orbital (HOMO-LUMO) of (SiO2)n clusters increase with size while the reverse is the norm in most clusters. The HOMO-LUMO gap decreases as the oxygen content of a SinOm cluster is lowered eventually approaching the visible range. The photoluminescence and strong size dependence of optical properties of small silica clusters could thus be attributed to oxygen defects.

Rights

Nayak, S. K., Rao, B. K., & Khanna, S. N., et al. Atomic and electronic structure of neutral and charged SinOm clusters. The Journal of Chemical Physics, 109, 1245 (1998). Copyright © 1998 American Institute of Physics.

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