Dielectric tensor and optical spectra of quaterthiophene crystals

We present an approach to the microscopic calculation of the dielectric tensor near the resonances of mechanical Frenkel excitons in a vibronic coupling regime with one effective mode. The model, applied to the prototypical quaterthiophene crystal, is based on a discrete distribution of charges for the evaluation of the molecular transition moment, whilst the coulombic interactions responsible for the exciton delocalization in the crystal are calculated by the Ewald method. From the calculated tensor we simulate absorbance and reflectance spectra and by a direct comparison with the experimental ones, we identify the origin of some shoulders present in the spectra.