Nanocrystalline Ni-Co alloys were synthesized using pulsed electrodeposition from a Watts-type bath, and the various plating parameters were systematically varied to examine their effect on the composition, quality, and structure of the resulting deposits. Increasing the pH of the plating bath and/or the average plating current density increased the Ni content of the deposits, but both of these parameters exhibited rather narrow processing windows for the preparation of high-quality deposits. The addition of saccharin during plating was observed both to reduce the crystallographic texture of the Ni-Co alloys and to refine the grain structure. Owing to the low stacking fault energy of Co, many of the alloy deposits exhibited a large density of nanoscale twins. The unique dual-scale grain and nano-twin structure found here caused apparent discrepancies in the grain size measured by XRD and by other microscopy techniques, and also resulted in unique trends in hardness. This thesis lays the groundwork for future tailoring of nanostructured alloys to explore how twins and stacking faults influence their strength and ductility.

The goals of this thesis were to synthesize nanocrystalline Zn, to study the mechanical properties of bulk nanocrystalline Zn and try to reveal the deformation mechanisms in nanocrystalline materials. Nanocrystalline Zn powder has been synthesized by a cryomilling method. The average grain size decreased exponentially with the cryomilling time and reached a minimum average grain size of around 17nm. Large numbers of small grains (2~6nm) have been found in the very early stages of cryomilling. Dynamic recrystallization (DRX) was used to explain the observed phenomena. Differential scanning calorimetry (DSC), x-ray diffraction and transmission electron microscopy (TEM) were used to study the structural changes and grain size distribution with milling time and subsequent annealing. Maxima in both stored enthalpy (for the low temperature DSC peak) and lattice strain on the Zn basal planes were observed at the same milling time. Dislocation density on the basal planes is proposed as a major source for lattice strain and the measured stored enthalpy. The released enthalpy that might be due to grain growth is very small. These cryomilled nanocrystalline Zn powders were consolidated into disks with a density of nearly theoretical density by uniaxial compression at room temperature. Cyclic variation of microhardness with milling time has been observed in cryomilled nanocrystalline Zn. Evidence from transmission electron microscopy (TEM) and high resolution transmission electron microscopy (HRTEM) suggests that the variation of dislocation density and grain size distributions determine the hardness behavior. A model, based on a kinetic reaction-rate model for cyclic amorphous-to-crystalline phase transformations observed during ball milling, simulates the experimental results very well. The model confirms the effect of DRX on modulated cyclic variation of microhardness. Dislocation strain hardening and recrystallization effects are superposed linearly with the intrinsic grain.