Inelastic neutron scattering experiments are combined with infrared and Raman data to obtain a uniquely defined description of the intramolecular vibrations of three oligomers of polythiophene, Through refinement of ab initio force fields, the three vibrational spectra of each oligomer are simulated with remarkable accuracy. Two different basis sets of atomic orbitals are used : the first, is 6-31G* and is used to optimize the geometries,and calculate the relevant force fields of alpha-2T and alpha-4T, the second is 3-21G* and is used for the same purpose for alpha-4T and alpha-6T. To improve agreement with the experiment, the force fields are scaled. In this way, one set of scaling parameters is generated for the 6-31G* basis and another for the 3-21G* basis. The parameters are common to both molecules calculated with either basis sets and are believed to be transferable to higher isomers, The fitting procedure is applied in steps : first, the calculated vibrational frequencies are assigned on the basis of the experimental infrared and Raman activity, then a fitting of the Inelastic Neutron Scattering profile is performed, finally, the infrared and Raman spectra are calculated with the new normal modes and the ab initio derivatives of the dipole moment and the polarizability. The procedure is iterated until the three spectra of each oligomer are satisfactorily reproduced. For alpha-4T, two scaled force fields are obtained-one for each basis set-and are shown to yield very similar normal modes. It is important to emphasize that not only the vibrational frequencies but also the spectral intensities are well reproduced by the simulations. Implicitly, this means that the dipole moment and the polarization tensor surfaces calculated nb initio at the potential energy surface minimum are of good quality. The procedure is absolutely general and can be applied to any molecular system. In the present case, it leads to well defined force fields that give us a stringent picture of the vibrations of these molecules.