Titanium dioxide thin films have been synthesized on Si (100) substrates using pulsed laser deposition method (KrF: 248 nm, 20 ns, 5 Hz). The emission spectra of the plasma induced by ablating TiO2 target in the oxygen or argon ambient gas were analyzed. The influences of substrate temperature and ambient gas pressure on the structural properties of TiO2 films were discussed. The X-ray diffraction results show that the films deposited at 750 degrees C are (004)-oriented anatase phase and (110)-oriented rutile phase under the oxygen and argon pressure of 5 Pa, respectively. The scanning electron microscopy images indicate that the TiO2 films have a uniform and smooth surface and are composed of nanocrystal grains. The pure anatase and rutile phase TiO2 films are further proved by Raman spectromicroscopy. In addition, the optical transmission spectra and Fourier Transform infrared spectroscopy of the films were also studied. (C) 2008 Elsevier B.V. All rights reserved.