Optical absorption spectra and geometric effects in higher fullerenes

TL;DR

This study theoretically investigates optical excitations in higher fullerenes, revealing how geometric arrangements of pentagons influence their optical spectra, with implications for understanding fullerene electronic properties.

Contribution

It introduces a detailed theoretical analysis of optical spectra in higher fullerenes considering geometric effects, using a tight binding model with Coulomb interactions.

Findings

Optical excitations below 4 eV are localized at pentagons.

Projected absorption spectra differ significantly from total absorption.

Spectral shapes are mainly determined by pentagon arrangements.

Abstract

The optical excitations in $\rug$ and higher fullerenes, including isomers of C$_{76}$, C$_{78}$, and C$_{84}$, are theoretically investigated. We use a tight binding model with long-range Coulomb interactions, treated by the Hartree-Fock and configuration-interaction methods. We find that the optical excitations in the energy region smaller than about 4 eV have most of their amplitudes at the pentagons. The oscillator strengths of projected absorption almost accord with those of the total absorption. When the projection is performed on each pentagon and pentagon dimers, the resultant spectrum in the low energy region is quite different from that of the total absorption. The spectral shapes of the total absorption are turned out to be determined mainly by the geometrical distributions of the pentagons in the fullerene structures.