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

Abstract

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