The electronic transport properties of polycrystalline pentacene-based thin film transistors (TFTs) were investigated at the microscopic level using microRaman spectroscopy. All the pentacene film, which were thermally evaporated as a layer with thickness of 70 nm, featured polycrystalline structure with only "thin film" phase polymorph and grain morphology as verified by x-ray diffraction (XRD) measurements. We have investigated the molecular vibrational modes of pentacene in the active channel during operations the organic TFT devices using in-situ Raman spectroscopy. Extra vibrational modes resulting from vibrational coupling effect in pentacene film were studied. The interlayer and intralayer intermolecular vibrational coupling energy was calculated from the Davydov splitting using a simple coupled-oscillator model. The results suggest that the C-H in-plane bending vibrational coupling energy of pentacene molecules in solid film is affected by operating device. Additionally, the aromatic C-C stretching vibrational modes also were investigated. However, it is rather difficult to obtain the variations of lattice parameters of pentacene film in a very small active channel by using electron diffraction and XRD. At the same time, MicroRaman technique provides the capability to explore the intermolecular coupling and molecular structure modifications.