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Journal Articles Scientific Reports Year : 2015

Unravelling the origin of the giant Zn deficiency in wurtzite type ZnO nanoparticles

Abstract

Owing to its high technological importance for optoelectronics, zinc oxide received much attention. In particular, the role of defects on its physical properties has been extensively studied as well as their thermodynamical stability. In particular, a large concentration of Zn vacancies in ZnO bulk materials is so far considered highly unstable. Here we report that the thermal decomposition of zinc peroxide produces wurtzite-​type ZnO nanoparticles with an extraordinary large amount of zinc vacancies (>15​%)​. These Zn vacancies segregate at the surface of the nanoparticles, as confirmed by ab initio calculations, to form a pseudo core-​shell structure made of a dense ZnO sphere coated by a Zn free oxo-​hydroxide mono layer. In others terms, oxygen terminated surfaces are privileged over zinc-​terminated surfaces for passivation reasons what accounts for the Zn off-​stoichiometry observed in ultra-​fine powdered samples. Such Zn-​deficient Zn1-​xO nanoparticles exhibit an unprecedented photoluminescence signature suggesting that the core-​shell-​like edifice drastically influences the electronic structure of ZnO. This nanostructuration could be at the origin of the recent stabilisation of p-​type charge carriers in nitrogen-​doped ZnO nanoparticles.
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hal-01194456 , version 1 (17-05-2024)

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Adèle Renaud, Laurent Cario, Xavier Rocquefelte, Philippe Deniard, Eric Gautron, et al.. Unravelling the origin of the giant Zn deficiency in wurtzite type ZnO nanoparticles. Scientific Reports, 2015, 5 (1), pp.12914. ⟨10.1038/srep12914⟩. ⟨hal-01194456⟩
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