Size-controlled silicon nanocrystals in silicon oxynitride matrix were prepared using plasma-enhanced chemical vapor deposition following the superlattice approach. A combination of current transport and charge trapping studies is carried out on a number of samples with varied structural configuration. We demonstrate that at low electric fields, trapping of injected carriers dominates, if the coupling between the silicon nanocrystals is strong. In contrast, we show that at higher electric fields, the charge distribution within the films is essentially governed by charge separation within the superlattice. This effect can be well explained by a two-step electric field ionization of silicon nanocrystals that proceeds via defect-assisted band-to-band tunneling of silicon valence electrons to the conduction band and is mediated by silicon surface dangling bonds. The defects are dominating the charge transport even if the defect density is reduced to a minimum by efficient hydrogen passivation.
Charge transport and electroluminescence mechanisms in Si-rich Si oxynitride/silicon oxide (SRON/SiO2) superlattices deposited on p-type Si substrate are reported. The superlattice structures were deposited by plasma-enhanced chemical-vapor deposition and subsequently annealed at 1150 °C to precipitate and crystallize the Si excess into Si nanocrystals. The dependence of the electrical conduction on the applied voltage and temperature was found to be well described by a Poole-Frenkel transport mechanism over a wide voltage range. On the other hand, the observed dependence of the electroluminescence on the SRON layer thickness is a clear proof of quantum confinement and was attributed to an excitonic radiative recombination taking place in the confined states within the Si quantum dots. A model is proposed based on thermal hopping of electrons between the quantum dots acting as trap states (Poole-Frenkel). A correlation between carrier transport and electroluminescence has been established considering impact ionization of high-kinetic energy electrons on the Si quantum dots
We study the electronic properties of phosphorus doped Si nanocrystal/SiO2 superlattices and determine the carrier concentration by transient current analysis. This is achieved by encapsulating the multilayers between two electrical insulation layers and controlling the carrier mobility by a defined layer to layer separation. A saturation of the voltage dependent ionized carrier density is observed which indicates complete substitutional dopant ionization and allows to calculate the dopant induced charge carrier density. It is found that the doping efficiency of the superlattice is only 0.12% considering the full ionization regime which explains the unusual small dopant effect on transport characteristics.
SummaryWe use high-temperature-stable silicon nitride membranes to investigate single layers of silicon nanocrystal ensembles by energy filtered transmission electron microscopy. The silicon nanocrystals are prepared from the precipitation of a silicon-rich oxynitride layer sandwiched between two SiO2 diffusion barriers and subjected to a high-temperature annealing. We find that such single layers are very sensitive to the annealing parameters and may lead to a significant loss of excess silicon. In addition, these ultrathin layers suffer from significant electron beam damage that needs to be minimized in order to image the pristine sample morphology. Finally we demonstrate how the silicon nanocrystal size distribution develops from a broad to a narrow log-normal distribution, when the initial precipitation layer thickness and stoichiometry are below a critical value.
This paper reports the growth of silicon nanocrystals (SiNCs) from SiH4-O-2 plasma chemistry. The formation of an oxynitride was avoided by using O-2 instead of the widely used N2O as precursor. X-ray photoelectron spectroscopy is used to prove the absence of nitrogen in the layers and determine the film stoichiometry. It is shown that the Si rich film growth is achieved via nonequilibrium deposition that resembles a interphase clusters mixture model. Photoluminescence and Fourier transformed infrared spectroscopy are used to monitor the formation process of the SiNCs, to reveal that the phase separation is completed at lower temperatures as for SiNCs based on oxynitrides. Additionally, transmission electron microscopy proves that the SiNC sizes are well controllable by superlattice configuration, and as a result, the optical emission band of the Si nanocrystal can be tuned over a wide range
Non-percolating and percolating silicon quantum dot (QD) networks were investigated by plane-view energy filtered transmission electron microscopy (EF-TEM). The Si QD networks were prepared by plasma enhanced chemical vapor deposition on free standing 5 nm Si3N4 membranes, followed by high temperature annealing. The percolation threshold from non-percolating to percolating networks is found to be in between a SiOx stoichiometry of SiO0.5 up to SiO0.7. Using the EF-TEM images, key structural parameters of the Si QD ensemble were extracted and compared, i.e., their size distribution, nearest neighbor distance, and circularity. Increasing the silicon excess within the SiOx layer results in an ensemble of closer spaced, less size-controlled, and less circular Si QDs that give rise to coupling effects. Furthermore, the influence of the structural parameters on the optical and electrical Si QD ensemble properties is discussed.
We report results of investigating carrier recombination in silicon nanocrystal/silicon dioxide superlattices. The superlattices prepared by nitrogen-free plasma enhanced chemical vapour deposition contained layers of silicon nanocrystals. Femtosecond transient transmission optical spectroscopy was used to monitor carrier mechanisms in the samples. The three-particle Auger recombination was observed in accord with previous reports. However, under high pump intensities (high photoexcited carrier densities) the bimolecular process dominated the recombination. Detailed analysis of measured data and fitting procedure made it possible to follow and quantify the interplay between the two recombination processes. The bimolecular recombination was interpreted in terms of the trap-assisted Auger recombination.
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