Ab initio angle- and energy-resolved photoelectron spectroscopy with time-dependent density-functional theory

摘要

We present a time-dependent density-functional method able to describe the photoelectron spectrum of atomsnand molecules when excited by laser pulses. This computationally feasible scheme is based on a geometricalnpartitioning that efficiently gives access to photoelectron spectroscopy in time-dependent density-functionalncalculations. By using a geometrical approach, we provide a simple description of momentum-resolvednphotoemission including multiphoton effects. The approach is validated by comparison with results in thenliterature and exact calculations. Furthermore, we present numerical photoelectron angular distributions fornrandomly oriented nitrogen molecules in a short near-infrared intense laser pulse and helium-(I) angular spectranfor aligned carbon monoxide and benzene.