We report Raman studies of GaAs and InAs nanowires (NWs) grown on SiO2 and GaAs surfaces by means of catalyst-assisted molecular beam epitaxy. We have investigated several tens of NWs grown using either Mn or Au as a catalyst. The LO and TO phonon lines of the NWs showed an energy downshift and a broadening as compared to the lines usually observed in the corresponding bulk materials. A doublet is sometimes observed in the LO region due to the observation of a signal attributed to the surface optical (SO) phonon. The energy position of the SO phonon agrees with the values expected considering the section diameter of the NWs. LO and TO downshifts are due to the presence of structural defects within the NWs. The larger the energy downshift, the smaller the dimension of the defect-free regions. The results demonstrate that different catalysts provide wires with comparable crystal quality. The measurements also point out that differences in defect density can be found in wires coming from the same batch indicating that a substantial effort will be needed to obtain high homogeneities of the NW quality.
Physical vapor deposition onto rare gas buffer layers leads to the spontaneous formation of clusters. During the thermal desorption of the buffer, these clusters diffuse and aggregate into larger structures, a process known as buffer-layer-assisted growth and desorption assisted coalescence. We studied the effect of buffer thickness and the rate of buffer desorption on the extent of this aggregation for Ag, Au, Cu, Pd, Co, and Ni particles on a solid Xe surface. On the basis of these experiments, results from Monte Carlo simulations and the existing theoretical models for cluster-cluster aggregation, we report for the first time the Arrhenius parameters for nanoparticle slip-diffusion. The effective activation energies range from 0.12 for small Ag clusters (few hundred atoms) to 0.60 eV for ramified Ni islands (millions of atoms), and the giant pre-exponential factors were found to differ by many orders of magnitude. Significantly, the pre-exponential factors follow a Meyer-Neldeltype dependence on the corresponding effective activation energy, with a characteristic Meyer-Neldel energy of 6.9 meV. This energy is associated with the phononic excitations in solid Xe that are responsible for nanostructure mobility. This dependence should be a characteristic feature of nanoparticle diffusion.
Physical vapor deposition of a wide range of materials on rare-gas solids leads to spontaneous cluster formation. Desorption of the rare-gas buffer causes the clusters to aggregate, a process known as buffer-layerassisted growth. We have studied the extent of aggregation and the size distribution of Au nanostructures as a function of the buffer composition ͑Xe, Kr, and Ar͒ and thickness, using transmission electron microscopy to image them after buffer desorption and delivery to amorphous carbon substrates. For small compact Au nanostructures ͑less than ϳ5 nm mean radius, р3ϫ10 4 atoms͒, the diffusivity varies strongly with size and even increases with average size in a limited range. This enhanced diffusion phenomenon is attributed to self-heating during coalescence. It is most important for small particles and is more evident on Kr than on Xe because of weaker interface coupling. In the limit of large ramified Au nanostructures ͑exceeding ϳ10 nm mean radius, у2ϫ10 5 atoms͒, the diffusivity scales as the inverse of the contact area, in agreement with molecular dynamics simulations of fast slip diffusion of nanocrystals on incommensurate surfaces. Motion is driven by phonons of the cluster and substrate, and is controlled by friction between a cluster facet and the buffer surface. A simple model is proposed that explains the observed exponential dependence of cluster size on buffer thickness. In this model, the growth kinetics are controlled by competition between the rate of cluster diffusion and the rate of buffer depletion.
Very recently, two-dimensional (2D) perovskite nanosheets (PNSs), taking the advantages of perovskite as well as the 2D structure properties, have received an enormous level of interest throughout the scientific community. In spite of this incredible success in perovskite nanocrystals (NCs), self-assembly of many nanostructures in metal halide perovskites has not yet been realized, and producing highly efficient red-emitting PNSs remains challenging. In this Letter, we show that by using CsPbBrI2 perovskite nanoparticles (NPs) as a building block, PNSs can emerge spontaneously under high ambient pressure via template-free self-assembly without additional complicated operation. It is found that the formation of PNSs is ascribed to the high pressure that provides the driving force for the alignment of NPs in solution. Because of the disappearance of the grain boundaries between the adjacent NPs and increased crystallinity, these PNSs self-assembled from NPs exhibit enhanced properties compared to the initial NPs, including higher PL intensity and remarkable chemical stability toward light and water.
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