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Article Dans Une Revue Nanoscale Advances Année : 2022

Modulating the growth of chemically deposited ZnO nanowires and the formation of nitrogen- and hydrogen-related defects using the pH adjustment

Résumé

ZnO nanowires (NWs) grown by chemical bath deposition (CBD) have received great interest for nanoscale engineering devices, but their formation in aqueous solution containing many impurities needs to be carefully addressed. In particular, the pH of the CBD solution and its effect on the formation mechanisms of ZnO NWs and of nitrogen-and hydrogen-related defects in their center are still unexplored. By adjusting its value in a low-and high-pH region, we show the latent evolution of the morphological and optical properties of ZnO NWs, as well as the modulated incorporation of nitrogenand hydrogen-related defects in their center using Raman and cathodoluminescence spectroscopy. The increase in pH is related to the increase in the oxygen chemical potential (µO), for which the formation energy of hydrogen in bond-centered sites (HBC) and VZn-NO-H defect complexes is found to be unchanged, whereas the formation energy of zinc vacancy (VZn) and zinc vacancy-hydrogen (VZn-nH) complexes steadily decreases as shown from density-functional theory calculations. Revealing that these VZn-related defects are energetically favorable to form as µO is increased, ZnO NWs grown in the high-pH region are found to exhibit a higher density of VZn-nH defect complexes than ZnO NWs grown in the low-pH region. Annealing at 450 °C under an oxygen atmosphere helps tuning the optical properties of ZnO NWs by reducing the density of HBC and VZn-related defects, while activating the formation of VZn-NO-H defect complexes. These findings show the influence of pH on the nature of Zn(II) species, the electrostatic interactions between these species and ZnO NW surfaces, and the formation energy of the involved defects. They emphasize the crucial role of the pH of the CBD solution and open new possibilities for simultaneously engineering the morphology of ZnO NWs and the formation of nitrogenand hydrogen-related defects.
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Dates et versions

hal-03623786 , version 1 (29-03-2022)

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Jose Villafuerte, Eirini Sarigiannidou, Fabrice Donatini, Joseph Kioseoglou, Odette Chaix-Pluchery, et al.. Modulating the growth of chemically deposited ZnO nanowires and the formation of nitrogen- and hydrogen-related defects using the pH adjustment. Nanoscale Advances, 2022, 4, pp.1793-1807. ⟨10.1039/d1na00785h⟩. ⟨hal-03623786⟩
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