Many-body photoemission theory for organic molecular crystals

Highlights: • We apply the Hedin equation to discuss the electron-phonon interaction. • Our framework gives a unified picture of the UPS spectra from organic solids. • We discuss the effects of multiple scatterings on the PAD. A many-body photoemission theory based on Keldysh nonequilibrium Green's functions is developed and applied to photoemission from extended states of organic molecules and their crystals, in particular excited by ultraviolet and soft X-ray radiation. In this energy region, electron-phonon interaction and radiation filed screening play some important roles. To incorporate the latter effects, we should use quantum electrodynamics (QED) approach. To discuss the electron-phonon interaction, we apply the Hedin equation including the screened Coulomb interaction mediated by the electron-phonon interaction. This theoretical framework gives us a unified picture of the UPS spectra from organic solids. Furthermore some illustrative numerical calculations are shown to discuss the relative importance of the multiple scatterings, Debye-Waller factors, the peak width of the quasi-particles, and the angular dependence of the phonon satellites. We demonstrate some specific features of ultraviolet photoemission spectroscopy (UPS) spectra from particularly anisotropic organic solids.