Generalized oscillator strength of endohedral molecules

TL;DR

This paper analyzes the inelastic electron scattering on endohedral molecules, specifically noble gas atoms inside fullerenes, using generalized oscillator strengths and considering effects of the fullerene shell's static potential and polarization.

Contribution

It introduces a model for calculating GOS in endohedral molecules considering static and polarization effects within the RPAE framework, extending previous atomic GOS studies to complex molecules.

Findings

Significant deviation from photoionization observed at small momentum transfer q.

Effects of fullerene shell's static potential and polarization are quantitatively characterized.

Analysis of onion-type endohedrals with nested fullerenes provided insights into complex structures.

Abstract

We investigate here the fast electron scattering upon endohedral atoms that present a fullerene CN staffed by an atom A, A@CN. We calculate the inelastic scattering cross-section expressing it via generalized oscillator strengths (GOS) density. We take into account two major effects of CN upon ionization of the atom A. Namely, the scattering of the electron by the static potential of the fullerenes shell and modification of the interaction between the fast incoming and atomic electrons due to polarization of the fullerenes shell by the incoming electron beam. To obtain the main features of the effect, we substitute the complex fullerenes shell CN by a static zero thickness potential, express its deformation under incoming electron action via CN polarizabilities. We perform all consideration in the frame of the so-called random phase approximation with exchange (RPAE) that gave reliable results for GOSes of isolated atoms, and expressions for absolute and differential in angle cross-sections. We limit ourselves with dipole and biggest non-dipole contributions to the differential in angle cross-section. We compare fast electron scattering with photoionization as a source of information on the target electronic structure and emphasize some advantages of fast electron scattering. As concrete objects of calculations, we choose noble gas endohedrals Ar@C60 and Xe@C60. The results are presented for two transferred momentum q values: q=0.1 and 1.0. Even for small q=0.1, in the so-called optical limit, the deviation from photoionization case is prominent and instructive. As an interesting and very specific object, we study onion-type endohedrals A@CN1@CN2, in which the all construction A@CN1 is stuffed inside CN2 with N2 >> N1.