Structural evolution of nanocrystalline silicon thin films synthesized in high-density, low-temperature reactive plasmas

Silicon thin films with a variable content of nanocrystalline phase were deposited on single-crystal silicon and glass substrates by inductively coupled plasma-assisted chemical vapor deposition using a silane precursor without any hydrogen dilution in the low substrate temperature range from 100 to 300 degrees C. The structural and optical properties of the deposited films are systematically investigated by Raman spectroscopy, x-ray diffraction, Fourier transform infrared absorption spectroscopy, UV/vis spectroscopy, scanning electron microscopy and high-resolution transmission electron microscopy. It is shown that the structure of the silicon thin films evolves from the purely amorphous phase to the nanocrystalline phase when the substrate temperature is increased from 100 to 150 degrees C. It is found that the variations of the crystalline fraction f(c), bonded hydrogen content C(H), optical bandgap E(Tauc), film microstructure and growth rate R(d) are closely related to the substrate temperature. In particular, at a substrate temperature of 300 degrees C, the nanocrystalline Si thin films of our interest feature a high growth rate of 1.63 nm s(-1), a low hydrogen content of 4.0 at.%, a high crystalline fraction of 69.1%, a low optical bandgap of 1.55 eV and an almost vertically aligned columnar structure with a mean grain size of approximately 10 nm. It is also shown that the low-temperature synthesis of nanocrystalline Si thin films without any hydrogen dilution is attributed to the outstanding dissociation ability of the high-density inductively coupled plasmas and effective plasma-surface interactions during the growth process. Our results offer a highly effective yet simple and environmentally friendly technique to synthesize high-quality nanocrystalline Si films, vitally needed for the development of new-generation solar cells and other emerging nanotechnologies.