Phase modulated Spectroscopic Ellipsometry (SE), in the spectral range from 1.5eV to 4.6eV, was employed to characterise thin film polysilicon (poly-Si) deposited by Low Pressure Chemical Vapour Deposition (LPCVD) on SiO2/Si(100) substrates as a function of process parameters. The LPCVD deposition temperature was varied from 550°C to 620°C for silane pressures ranging from 100mTorr to 230mTorr. A variation in poly-Si microstructure was observed as a function of film depth. The influence of deposition conditions on poly-Si surface morphology was quantified using both atomic force microscopy (AFM) and SE. An increase in the measured Raman TO phonon amplitude was observed for the 620°C sample set as a function of increasing LPCVD process pressure.