Ab initio calculation of the electronic and optical properties of solid pentacene -: art. no. 115212

The optical and electronic properties of crystalline pentacene are studied, using a first-principle Green's-function approach. The quasiparticle energies are calculated within the GW approximation and the electron-hole excitations are computed by solving the Bethe-Salpeter equation. We investigate the role of polymorphism on the electronic energy gap and linear optical spectrum by studying two different crystalline phases: the solution-phase structure and the vapor-phase structure. Charge-transfer excitons are found to dominate the optical spectrum. Excitons with sizable binding energies are predicted for both phases.