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

TL;DR

This paper introduces a computationally efficient time-dependent density-functional method for simulating angle- and energy-resolved photoelectron spectra of atoms and molecules under laser excitation, including multi-photon effects.

Contribution

It presents a novel geometrical partitioning approach enabling accurate and feasible simulations of photoelectron spectra within time-dependent density-functional theory.

Findings

Validated method against literature and exact results

Generated numerical photoelectron angular distributions for molecules and atoms

Demonstrated multi-photon effects in photoemission spectra

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 photoe- mission including multi-photon 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.