A method of depositing and crystallizing materials on a substrate is disclosed. In a particular embodiment, the method may include creating a plasma having deposition-related species and energy-carrying species. During a first time period, no bias voltage is applied to the substrate, and species are deposited on the substrate via plasma deposition. During a second time period, a voltage is applied to the substrate, which attracts ions to and into the deposited species, thereby causing the deposited layer to crystallize. This process can be repeated until an adequate thickness is achieved. In another embodiment, the bias voltage or bias pulse duration can be varied to change the amount of crystallization that occurs. In another embodiment, a dopant may be used to dope the deposited layers.