Si nanoclusters embedded in SiO2 have been produced by thermal annealing of SiOx films prepared by plasma enhanced chemical vapor deposition. The structural properties of the system have been investigated by energy filtered transmission electron microscopy (EFTEM). EFTEM has evidenced the presence of a relevant contribution of amorphous nanostructures, not detectable by using the more conventional dark field transmission electron microscopy technique. By also taking into account this contribution, an accurate quantitative description of the evolution of the samples upon thermal annealing has been accomplished. In particular, the temperatures at which the nucleation of amorphous and crystalline Si nanoclusters starts have been determined. Furthermore, the nanocluster mean radius and density have been determined as a function of the annealing temperature. Finally, the optical and the structural properties of the system have been compared, to demonstrate that the photoluminescence properties of the system depend on both the amorphous and crystalline clusters.
We provide a semi-empirical model based on in situ degradation measurements to predict the durability of hybrid perovskite materials under simulated thermal operation conditions. In the model, the degradation path of MAPbI3 layers is proved to follow an Arrhenius-type law. The predictive role is played by the activation energy combined with its pre-exponential factor. Our comparative study under moisture conditions with respect to vacuum and nitrogen treatments has assessed the occurrence of an intrinsic dynamic exchange of protons between the organic cations and the inorganic cage with a direct impact on the lattice stability, for which the presence of water molecules is not mandatory. This mutual interaction produces defects inside the material and volatile species, such as HI, CH3NH2 or MAI, with an associated experimental activation energy of 1.54 eV measured under vacuum conditions in dark. This value is comparable to that calculated by the density functional theory for defect generation in MAPbI3. In air, the action of water molecules reduces the activation energy for proton exchanges in dark to 0.96 eV. As an alternative solution to increase the material stability, we demonstrate that the substitution of methylammonium (MA(+)) with the formamidinium (FA(+)) cations inside the inorganic cage gives greater robustness to the overall lattice and extends the material durability due to a different interaction between the organic molecules and the inorganic cage. This definitely supports the use of FAPbI3 in applications, provided its structure can be stabilized in the dark phase at room temperature.
We report the synthesis, the structural and optical characterization of CdSe/CdS/ZnS "double shell" nanorods and their exploitation in cell labeling experiments. To synthesize such nanorods, first "dot-in-a-rod" CdSe(dot)/CdS(rod) core/shell nanocrystals were prepared. Then a ZnS shell was grown epitaxially over these CdSe/CdS nanorods, which led to a fluorescence quantum yield of the final core-shell-shell nanorods that could be as high as 75%. The quantum efficiency was correlated with the aspect ratio of the nanorods and with the thickness of the ZnS shell around the starting CdSe/CdS rods, which varied from 1 to 4 monolayers (as supported by a combination of X-ray diffraction, elemental analysis with inductively coupled plasma atomic emission spectroscopy and high resolution transmission electron microscopy analysis). Pump-probe and time-resolved photoluminescence measurements confirmed the reduction of trapping at CdS surface due to the presence of the ZnS shell, which resulted in more efficient photoluminescence. These double shell nanorods have potential applications as fluorescent biological labels, as we found that they are brighter in cell imaging as compared to the starting CdSe/CdS nanorods and to the CdSe/ZnS quantum dots, therefore a lower amount of material is required to label the cells. Concerning their cytotoxicity, according to the MTT assay, the double shell nanorods were less toxic than the starting core/shell nanorods and than the CdSe/ZnS quantum dots, although the latter still exhibited a lower intracellular toxicity than both nanorod samples.
Light-emitting silicon nanocrystals embedded in SiO 2 have been investigated by x-ray absorption measurements in total electron and photoluminescence yields, by energy filtered transmission electron microscopy and by ab initio total energy calculations. Both experimental and theoretical results show that the interface between the silicon nanocrystals and the surrounding SiO 2 is not sharp: an intermediate region of amorphous nature and variable composition links the crystalline Si with the amorphous stoichiometric SiO 2. This region plays an active role in the light-emission process.
In this letter, the role of amorphous Si clusters in the excitation of Er implanted in substoichiometric SiOx films will be elucidated. It will be shown that the temperature of the SiOx thermal process prior to Er implantation is crucial in determining the luminescence properties of the samples. In particular, the luminescence intensity at 1.54 μm is almost constant for SiOx samples not annealed or pre-annealed at temperatures lower than 800 °C, reaches the maximum at 800 °C, and decreases at higher temperatures. The structural properties of these samples have been studied by energy filtered transmission electron microscopy. It will be shown that for annealing temperatures lower than 1000 °C, only amorphous Si nanoclusters are present. We demonstrate that a large density of small amorphous Si clusters produces the best luminescence performance and enhances the fraction of optically active Er.
We present a novel approach for the direct synthesis of ultrathin Si nanowires (NWs) exhibiting room temperature light emission. The synthesis is based on a wet etching process assisted by a metal thin film. The thickness-dependent morphology of the metal layer produces uncovered nanometer-size regions which act as precursor sites for NW formation. The process is cheap, fast, maskless and compatible with Si technology. Very dense arrays of long (several micrometers) and small (diameter of 5-9 nm) NWs have been synthesized. An efficient room temperature luminescence, visible with the naked eye, is observed when NWs are optically excited, exhibiting a blue-shift with decreasing NW size in agreement with quantum confinement effects. A prototype device based on Si NWs has been fabricated showing a strong and stable electroluminescence at low voltages. The relevance and the perspectives of the reported results are discussed, opening the route toward novel applications of Si NWs.
The enhanced diffusion of donor atoms, via a vacancy (V)-mechanism, severely affects the realization of ultrahigh doped regions in miniaturized germanium (Ge) based devices. In this work, we report a study about the effect of fluorine (F) on the diffusion of arsenic (As) in Ge and give insights on the physical mechanisms involved. With these aims we employed experiments in Ge co-implanted with F and As and density functional theory calculations. We demonstrate that the implantation of F enriches the Ge matrix in V, causing an enhanced diffusion of As within the layer amorphized by F and As implantation and subsequently regrown by solid phase epitaxy. Next to the end-of-range damaged region F forms complexes with Ge interstitials, that act as sinks for V and induce an abrupt suppression of As diffusion. The interaction of Ge interstitials with fluorine interstitials is confirmed by theoretical calculations. Finally, we prove that a possible F-As chemical interaction does not play any significant role on dopant diffusion. These results can be applied to realize abrupt ultra-shallow n-type doped regions in future generation of Ge-based devices.
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