We have investigated the electronic structures of recently discovered superconductor FeSe by soft-x-ray and hard-x-ray photoemission spectroscopy with high bulk sensitivity. The large Fe 3d spectral weight is located in the vicinity of the Fermi level (EF ), which is demonstrated to be a coherent quasi-particle peak. Compared with the results of the band structure calculation with local-density approximation, Fe 3d band narrowing and the energy shift of the band toward EF are found, suggesting an importance of the electron correlation effect in FeSe. The self energy correction provides the larger mass enhancement value (Z −1 ≃3.6) than in Fe-As superconductors and enables us to separate a incoherent part from the spectrum. These features are quite consistent with the results of recent dynamical mean-field calculations, in which the incoherent part is attributed to the lower Hubbard band.
The formation of nanoscale fine structures during pulsed laser ablation of a silicon target in a hydrogen atmosphere has been studied by analyzing the deposited silicon fine structures prepared under different conditions. Transmission electron microscopy, scanning electron microscopy ͑SEM͒, Raman scattering, and infrared absorption studies on the deposited samples indicate that silicon nanocrystallites are produced when the background gas pressure is higher than a critical value. The deposited substance is found to show hierarchical structure having surface hydrogenated silicon nanocrystallites as the primary structure and aggregates of the nanocrystallites as the secondary structure. The secondary structure depends on the hydrogen background gas pressure, while the size of the primary nanocrystallites is 4 -5 nm independent of the pressure. These results suggest that the fine structure is formed in two steps; the silicon nanocrystallites having a stable surface are initially formed and they are subsequently aggregated to form the secondary structure. Analysis of surface free energy suggests that the stability is acquired by termination of the surface by creation of Siu H bonds. We carried out fractal analysis of the SEM image of the deposits and found that the secondary structure shows good self-similar structure when deposited at higher background gas pressure. The fractal dimension of aggregated secondary structure varies from 1.7 to more than 2.0 with decreasing background gas pressure. Comparison of these values with reported results for the fractal growth simulation indicates that the region at which aggregation of the nanocrystallites takes place changes from in the plume to on the substrate with decreasing background gas pressure. Effects of the hydrogen background gas on the nanocrystallization process and spatial distribution of formed nanocrystallites in the plume are discussed. The formation of surface stabilized Si nanocrystallites and their spatial confinement by background gas in the first and second steps determine the hierarchical structure of deposited substance.
Abstract. We performed pulsed laser ablation (PLA) of a silicon target in liquid environment to prepare a silicon colloid solution. The nanoparticles were observed by SEM and TEM measurements. The result of Raman scattering indicates that this particle is mainly composed of silicon nanocrystallites. The optical gap energies of the colloid solutions varied by changing the solvents; 2.9 and 3.5 eV for colloids prepared in water and hexane, respectively. These colloid solutions showed efficient PL intensity. Since Si-(CH 3 ) n related bonds were observed for the specimen prepared in hexane, surface effects other than the quantum confinement effect should be taken into account for the origin of the PL. Our results indicate that new kinds of Sibased colloid solutions can be prepared by PLA in solvent. Since the PL peak energies were sensitive to the surface conditions, these colloid solutions are promising for biological applications such as bio-sensors.
Natural oxidation processes of surface hydrogenated silicon nanocrystallites prepared by pulsed laser ablation under various hydrogen gas pressures are discussed by measuring the vibrational frequency of Si-H n units on the surface and intensity of Si-O-Si stretching vibration. The surfaces of nanocrystallites are predominantly composed of Si-H bonds and oxidation starts from backbonds of these bonds. The deposited nanocrystal films have a porous secondary structure which depends on the background gas pressure. The oxidation rate observed by infrared absorption measurements depended on this porous secondary structure. The oxidation process is discussed by the correlation between oxidation rate and porous structure of nanocrystal film. We found that Si-O bond density increases with covering the surface of the nanocrystallites during the diffusion of oxygen-related molecules through the void spaces in the porous structure. The surface oxidation of each nanocrystallite is not homogeneous; after the coverage of easy-to-oxidize sites, oxidation continues to gradually progress at the post-coverage stage. We point out that the oxidation process at coverage and post-coverage stages result in different photoluminescence ͑PL͒ wavelengths. Adsorption of the water molecule before oxidation also affects the PL wavelength. Defect PL centers which have light emission around 600 and 400 nm are generated during the coverage and post-coverage oxidation processes, respectively.
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