Papers by Author: Michael Bruns

Abstract: Studies of self-diffusion in solids are presented, which are based on neutron reflectometry. For the application of this technique the samples under investigation are prepared in form of isotope heterostructures. These are nanometer sized thin films, which are chemically completely homogenous, but isotope modulated. Using this method, diffusion lengths in the order of 1 nm and below can be detected which allows to determine ultra low diffusivities in the order of 10-25 m2/s. For the model system amorphous silicon nitride we demonstrate how the structure of the isotope hetrostructures (triple layers or multilayers) influences the efficiency of diffusivity determination.

Abstract: The self-diffusion of nitrogen is studied in amorphous silicon nitride, which is a model system for a covalently bound amorphous solid with a low atomic mobility where reliable diffusion data are still lacking. Comparative experiments on Si14Nx/Si15Nx (x ≈ 1.33) isotope multilayers were carried out with secondary ion mass spectrometry (SIMS) and neutron reflectometry (NR), respectively. It was found that experiments with SIMS are not very well suited for the determination of diffusivities in a broad temperature range. The minimum diffusion length of about 5-10 nm detectable with this method is too large. At high temperatures (> 1200 °C) the amorphous solid crystallizes before any diffusion is measured and at low temperatures (< 1100 °C) the diffusivities are too low to be detected. In contrast, with neutron reflectometry diffusion lengths in the order of 1 nm and diffusivities down to 10-24 m2 s-1 were measured between 950 and 1250 °C. The potential of this method for the determination of ultra slow diffusion processes is discussed.

Abstract: The self-diffusion of nitrogen is investigated in polycrystalline thin silicon nitride films using a gas-exchange method (14N2/Si3 15N4) in comparison to Si3 14N4/Si3 15N4/Si3 14N4 isotope heterostructures. The films are produced by reactive r. f. magnetron sputtering. Depth profile analysis is carried out with secondary ion mass spectrometry (SIMS), secondary neutral mass spectrometry (SNMS), and nuclear resonant reaction analysis (NRRA). The nitrogen diffusivities determined with the use of isotope heterostructures follow an Arrhenius law in the temperature range between 1200 and 1700 °C with an activation enthalpy of DH = 4.9 eV and a pre-exponential factor of D0 = 1 x 10-6 m2/s, indicating a conventional diffusion mechanism via localized point defects. Using the gas-exchange method, the nitrogen diffusivities could be obtained only in the temperature range between 1600 and 1700 °C. This is due to the fact that at temperatures below 1600 °C the surface exchange process with its high activation enthalpy (about 10 eV) is rate limiting, leading to non detectable diffusion profiles. The application of the different methods of depth profiling leads to the same diffusivities within estimated errors.