Deposition of hafnium silicate films with various hafnium contents was tried by plasma-enhanced chemical vapor deposition using tetraethoxysilane and a hafnium alkoxide. From x-ray photoelectron spectroscopy, the deposited films are confirmed to be silicate with Hf–O–Si bonds but without any Hf–Si bonds. The permittivity calculated from the capacitance of the accumulation layer increases monotonically with an increase in the hafnium content, whereas the optical band gap energy estimated from vacuum ultraviolet absorption spectra decreases. Similar results were obtained from zirconium silicate films deposited using tetraethoxysilane and a zirconium alkoxide. If we compare the films with the same hafnium or zirconium content, the hafnium silicate exhibits a higher permittivity and a larger band gap energy than the zirconium silicate.
Hafnium and zirconium silicate films were deposited on a silicon substrate and the effects of postannealing on their electrical properties were investigated. When the films are postannealed in nitrogen monoxide (NO), the leakage current becomes lower by more than one order of magnitude as compared with that of the as-deposited films. The capacitance-voltage (C-V) hysteresis width is also decreased drastically by the NO postannealing. From electron spin resonance spectroscopy, it is indicated that paramagnetic defects at the interface between the film and the substrate are responsible for the leakage current and the C-V hysteresis. It is also indicated by x-ray photoelectron spectroscopy that the postnitridation effectively terminates these interface defects and contributes to the improvement in electrical properties.
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