The visible luminescence mechanism of ZnO is an important but controversial problem. In this paper, we report the structural and optical properties of Mg-doped ZnO nanoparticles (approximately 3-4 nm) synthesized via the sol-gel method. X-ray diffraction (XRD) analysis and absorption spectra observations revealed that Mg ions replace Zn ions in the lattice. In the room temperature photoluminescence (PL) spectra, three emission bands, ultraviolet (UV), blue, and green, were observed. With increasing concentration of Mg, the near band edge (NBE) emission band progressively shifted to the higher energy side. The green emission in the visible emission band, however, presented an inconspicuous shift. The reason is probably that the bottom of the conduction band in ZnO is determined by the Zn 4s state, and the top of the valence band is determined by the O 2p state. Mg ions in ZnO substitute for zinc ions and enter a slightly distorted tetrahedral site, which causes the bottom of the ZnO conduction band to be shifted to higher energy and leaves the top of the valence band unchanged. This combined with the fact that the deep level position is insensitive to the shift of the band edge led us to conclude that the green emission originates from electronic transition between the deep defect level and the top of the valence band (or very shallow acceptor level).
We presented our investigations on the absorption and emission properties of the nanocrystalline ZnO particles of different particle sizes (2 nm-5 nm) by sol-gel method. In the room temperature PL spectra, three emission bands, ultraviolet (UV), blue and green were observed. With increasing the particle sizes, both the UV and the visible emission bands shifted to lower energies progressively. From the size-dependency, there was a linear relationship between the energetic maxima of the UV and the green emission bands with a slope of about 0.26, which indicated that the green luminescence of ZnO was produced by the transitions of electrons from deep level to the valence band (or shallow acceptor level). A linear dependence was also found between the energetic maxima of the UV and the blue emissions with a slope of 0.15, the origin this blue emission band is not clear at present. While in van Dijken et al.'s paper, however, they identified only two emission bands in the emission spectra, an UV and a broad visible emission band, and the linear fit between the energetic maxima of these two bands in particles of different sizes has a slope of 0.6, so they proposed that the visible emission in ZnO was originated from the recombination of a shallowly trapped electron with a deeply trapped hole. We attributed this divergence to the fact that the broad visible band is actually composed of two separate emission bands originated from two different recombination processes, and should not had been treated as one emission band.
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