Higher Nanoparticle Volume Fraction Research Articles

Substrate temperature dependence of electrical conduction in nanocrystalline CdTe:TiO2 sputtered films

Abstract TiO2 thin films with high volume fraction (∼50­70 %) of CdTe nanoparticles were prepared by radio frequency (rf) magnetron sputtering from a composite TiO2:CdTe target. With increase in substrate temperature Ts from room temperature (RT ∼300 K) to 373 K, a transition from an ordered structure exhibiting metallic-type conduction to a disordered structure exhibiting nonmetallic-type conduction was observed for annealed nanocrystalline CdTe:TiO2 films. The annealed RT-deposited films showed a large coalescence of distinct islands (size ∼0.3­0.7 µm) mainly of Cd and CdTe, and as result, a 3D network was realized. For metallic regime films, electrical conduction is essentially due to electrical percolation through Cd/CdTe crystallites embedded in an amorphous TiO2 matrix. However, the annealed high Ts films consisted of noncoalescent, small islands (size ∼0.15­0.3 µm) of Cd and CdTe embedded in amorphous TiO2 matrix. Here, the conduction is essentially by hopping mechanism via thermally activated tunneling.

Nanoparticle Engineering of Complex Fluid Behavior

A new mechanism for regulating the stability of colloidal suspensions has been discovered, known as nanoparticle haloing.1 Colloidal microspheres suspended under conditions near their isoelectric point were stabilized by the addition of highly charged nanoparticles. Such species segregated to regions near negligibly charged microspheres leading to their effective charge buildup. At even higher nanoparticle volume fractions, system stability was reversed due to attractive depletion interactions. By engineering the strength of energetic and entropic interactions via nanoparticle additions, we have assembled colloidal fluid, gel, and crystalline phases from binary mixtures of colloidal silica microspheres and hydrous zirconia nanoparticles whose structure and flow behavior vary dramatically.

OPTICAL NONLINEARITIES OF METAL-DIELECTRIC COMPOSITES

Nonlinear optical properties of metal-dielectric composites, such as fractal colloid aggregates and clusters created by ion implantation, are studied. Strong fluctuations of local fields result in huge enhancements of optical nonlinearities in fractal colloid aggregates. The real and imaginary parts of the cubic susceptibility of silver colloid aggregates are measured. It is found that the coefficient of nonlinear absorption strongly depends on the laser wavelength and intensity. Optical limiting effect in fractal silver colloids is observed. Nondegenerate forward four-wave mixing technique is used to investigate the third-order nonlinear susceptibility for nanocomposite material with Au nanocrystals formed inside a SiO 2 glass matrix. The Au nanocrystals are formed by the ion implantation and annealing method that produces very high volume fraction of nanoparticles. The large value |χ(3)|=1.3×10-7 esu is measured. Two characteristic relaxation times, 5.3 ps and 0.66 ps, are estimated from the detuning curve of |χ(3)|, as the probe beam wavelength changes. A novel class of optical materials, microcavities doped with nanostructured fractal aggregates, is also studied. In our experiments, lasing at extremely low pump intensities, below 1 mW, and dramatically enhanced Raman scattering was observed in microcavity/fractal composites.