Many-body theory for angular resolved photoelectron spectra of metal clusters

TL;DR

This paper develops a many-body theoretical framework using the jellium model to accurately describe the angular resolved photoelectron spectra of sodium clusters, highlighting the importance of many-body effects and aligning well with experimental results.

Contribution

It introduces a comprehensive many-body theory for metal cluster photoelectron spectra, surpassing single particle approximations and matching experimental observations.

Findings

Many-body effects dominate the angular distributions of photoelectrons.

The theory accurately reproduces experimental spectra for Na7- and Na19- clusters.

Single particle models fail to explain the observed phenomena.

Abstract

Angular resolved photoelectron spectra of metal clusters have been experimentally measured for the first time only recently. These measurements have been performed systematically for sodium clusters in a broad range of cluster sizes. This work attracted a lot of attention and was reported practically at all major international cluster conferences because it revealed a very non-trivial behavior of the angular anisotropy parameter with respect to photon energy and provided a method for probing the angular momentum character of the valence orbitals of free nanoclusters. Initial attempts to explain these observations within single particle approximations fail completely. In this Letter we present a consistent many-body theory for the description of angular resolved photoelectron spectra of metal clusters. Jellium model formalism is employed. Our calculations demonstrate the dominant role of the many-body effects in the formation of angular distributions of photoelectrons emitted from sodium clusters and are in a good agreement with experimental data reported in. The concrete comparison of theory and experiment has been performed for the photoionization of $Na_7^{-}$ and $Na_{19}^{-}$ anions being characterized by the entirely closed shells of delocalized electrons.