Stabilized-jellium description of neutral and multiply charged fullerenes

TL;DR

This paper models neutral and charged fullerenes using a stabilized jellium approach combined with shell correction and local density approximation, successfully predicting energies, spectra, and stability consistent with experiments.

Contribution

It introduces a stabilized jellium model with shell correction for fullerenes, providing accurate predictions of energies, spectra, and charging behaviors.

Findings

Calculated single-particle energy levels match experimental data.

Charging energies for up to 12 excess charges are computed.

Doubly charged negative ion is metastable and long-lived.

Abstract

A description of neutral and multiply charged fullerenes is proposed based on a stabilized jellium (structureless pseudopotential) approximation for the ionic background and the local density approximation for the sigma and pi valence electrons. A recently developed shell-correction method is used to calculate total energies and properties of both the neutral and multiply charged anionic and cationic fullerenes. The effect of the icosahedral symmetry is included perturbatively. The calculated single-particle energy level spectrum of C_60 is in good correspondence with experimentally measured ones and previous self-consistent local-density-approximation calculations. For the multiply charged fullerenes, we calculate microscopically the charging energies for up to 12 excess charges. A semiclassical interpretation of these results is developed, which views the fullerenes as Coulomb islands possessing a classical capacitance. The calculated values for the first ionization potential and the first electron affinity agree well with the experimental ones. Our calculations support the results from charge transfer bracketing experiments and from direct ionization experiments through electron impact. The doubly charged negative ion is found to be a very long-lived metastable species, in agreement with observations.