Novel uniform-sized, core-shell ZnO mesocrystal microspheres have been synthesized on a large scale using a facile one-pot hydrothermal method in the presence of the water-soluble polymer poly(sodium 4-styrenesulfonate). The mesocrystal forms via a nonclassical crystallization process. The intrinsic dipole field introduced by the nanoplatelets as a result of selective adsorption of the polyelectrolyte on some polar surfaces of the nanoparticles acts as the driving force. In addition, it plays an important role throughout the mesoscale assembly process from the creation of the bimesocrystalline core to the apple-like structure and finally the microsphere. Our calculation based on a dipole model confirms the dipole-field-driven mechanism forming the apple-like structure.
Vacancy structures in tin oxide nanoribbons fabricated via thermal evaporation and post-processing are probed by luminescence spectroscopy, and interesting properties that bode well for oxygen sensing are observed. Besides a broad 620-nm band, the fabricated tin oxide nanoribbons show a photoluminescence band at 480 nm when the measurement temperature is <100 K. The blue band appears from nanoribbons synthesized under high oxygen pressure or annealed under oxygen. The dependence suggests that the oxygen interstitial and vacancy densities determine the electronic states that produce the blue band. Calculation of the electron structures based on the density functional theory shows that decreased oxygen vacancies or increased oxygen interstitials enhance the 480-nm band but suppress the 620-nm band. The results reported here indicate that the tin oxide nanoribbons with vacancy structures have potential applications in luminescence-sensitive oxygen sensing.
Amorphous ZnO granular films were fabricated by anodizing zinc sheet in 0.5M oxalic acid solution under direct current voltage. The photoluminescence spectrum of the as-anodized sample shows a very broad visible emission band, which can be Gaussian divided into two subbands at 525 and 600nm. Based on their annealing behavior and the growing mechanism of the ZnO films, the two subbands are attributed to optical transitions in oxygen vacancies and oxygen interstitials, respectively. Obvious redshifts of the two subbands were observed with increasing excitation wavelength. Spectral analyses suggest that the excitation wavelength dependences of the two subbands are due to the quantum confinement on the amorphous ZnO nanoparticles mainly with sizes of ∼10nm. This work provides a good understanding of the photoluminescence behavior of amorphous ZnO particles.
Raman scattering was performed on Ge x Si 1−x ͑x = 0.54 or 0.28͒ alloy nanocrystals embedded in amorphous Si oxide. An asymmetric, depolarized, and size-dependent low-frequency Raman peak was observed and identified as the superposition of two surface acoustic vibration modes of the alloy nanocrystals. The current theoretical models can be used to explain the mode frequencies but not the dampings observed experimentally. Based on energy-dispersive x-ray microanalysis and density-functional-theory total energy optimization of structures, a modified core-shell-matrix model in which the effects of neighboring nanocrystals in the matrix are taken into account is in good agreement with experiments. This work provides good insight into the frequencies and dampings of acoustic vibrations of the nanocrystals embedded in the matrix.
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