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Studies of diamond nucleation and growth were conducted with molecular and ionic gas species in an ultra-high vacuum system. Thermal interactions of C{dollar}\\rm\\sb2H\\sb4{dollar} on Si(100) 2 x 1 surfaces held at 1000 K produced carbon films comprised of SiC, sp{dollar}\\sp2{dollar}-C, and sp{dollar}\\sp3{dollar}-C, as determined using Auger electron spectroscopy. The presence of elemental Si on the surface throughout the growth process indicated that a surfactant mediated growth process, with Si as the surfactant, was responsible for both SiC and sp{dollar}\\sp3{dollar}-C growth. The presence of sp{dollar}\\sp2{dollar}-C in the films was most likely due to interfacial strain effects. Medium energy (500 eV) methyl and ethyl ion interactions with Si(100) surfaces held at 300 and 1000 K showed that these ions are more efficient than their molecular counterparts for producing sp{dollar}\\sp3{dollar}-C. That is, lower ion fluences were required to obtain comparable amounts of sp{dollar}\\sp3{dollar}-C in the growing films. Hydrogen ion interactions with SiC films produced carbon rich surfaces composed of sp{dollar}\\sp2{dollar}-C and sp{dollar}\\sp3{dollar}-C. The relative amounts of each carbon species were found to be strongly energy dependent. The formation of sp{dollar}\\sp3{dollar}-C required hydrogen ion energies in excess of that required for lattice displacements. These results suggest that two novel growth processes which may allow the deposition of epitaxial diamond films suitable for microelectronic applications.