The electronic structure of the neutral TTF molecule has been determined by the overlapping atomic sphere version of the self-consistent statistical exchange multiple scattering method. The radii of the overlapping atomic spheres were determined semi-empirically. The calculated energy level spectrum gives a satisfactory account of the optical spectrum of TTF molecules in solution, and of the photoemission spectra of TTF vapor and solid TTF. Symmetry assignments are provided for the principal energy levels. © 1975.