Abstract

AbstractIn this paper we present time‐dependent, quantum‐dynamical simulations of photoinduced processes at solid surfaces involving nonadiabatic transitions of electrons to and from short‐lived intermediate excited states. In particular, two‐photon photoemission (2PPE) spectra of naked metal surfaces and free‐standing metal films are considered. One major problem in both cases is the presence of electron—electron scattering, which is treated here in various ways. The first way is to adopt an open‐system density matrix approach, in which a single electron is weakly coupled to a “bath” of other electrons. The second approach is based on a many‐electron Schrödinger equation, which is solved with the help of a time‐dependent configuration interactions singles (TD—CIS) method.

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