We report on the growth and properties of novel amorphous Silicon (a-Si:H) p-i-n devices prepared using chemical annealing with argon gas. The i layer in the p-i-n devices was grown using a layer by layer approach, where the growth of a very thin a-Si:H layer (7-30 angstroms) grown using a silane:argon mixture was followed by chemical anneal by argon ions. Repeated cycling of such growth/anneal cycles was used to produce the desired total thickness of the i layer. The thickness of the a-Si layer, and duration of the anneal time, were varied systematically. Pressure and power of the plasma discharge were also systematically varied. It was found that a thin a-Si layer, <10 angstroms, and low pressures which led to relatively high ion flux on the surface, gave rise to a significantly smaller bandgap in the device, as indicated by a significant lateral shift in the quantum efficiency vs. photon energy curve to lower energies. The smallest Tauc gap observed was in the range of 1.62 eV. Corresponding to this smaller bandgap, the current in the solar cell increased, and the voltage decreased. The Urbach energies of the valence band tail were also measured in the device, using the quantum efficiency vs. energy curve, and found to be in the range of45 meV, indicating high quality devices. Too much ion bombardment led to an increase in Urbach energy, and an increase in defect density in the material. Raman spectra of the device i layer indicated an amorphous structure. When hydrogen was added to argon during the annealing cycle, some materials turned microcrystalline, as indicated by the Raman spectrum, and confirmed using x-ray diffraction.