Optical absorption spectra in fullerenes C60 and C70: Effects of Coulomb interactions, lattice fluctuations, and anisotropy

TL;DR

This paper theoretically investigates how Coulomb interactions, lattice fluctuations, and anisotropy influence the optical absorption spectra of fullerenes C60 and C70, achieving good agreement with experimental observations.

Contribution

It introduces a comprehensive model incorporating Coulomb interactions, bond disorder, and anisotropy effects to accurately simulate fullerene optical spectra.

Findings

Broad peaks in C60 spectra are well described by the model.

Lattice fluctuations cause broadening of spectral peaks.

Optical gap in C70 depends on molecular orientation.

Abstract

Effects of Coulomb interactions and lattice fluctuations in the optical absorption spectra of C60 and C70 are theoretically investigated by using a tight binding model with long-range Coulomb interaction and bond disorder. Anisotropy effects in C70 are also considered. Optical spectra are calculated by using the Hartree-Fock approximation followed by the configuration interaction method. The main conclusions are as follows: (1) The broad peaks at excitation energies, 3.7eV, 4.7eV, and 5.7eV, observed in experiments of C60 molecules in a solution are reasonably described by the present theory. Peak positions and relative oscillator strengths are in overall agreement with the experiments. The broadening of peaks by lattice fluctuations is well simulated by the bond disorder model. (2) The optical gap of C70 is larger when the electric field of light is parallel to the long axis of the molecule. The shape of the frequency dispersion also depends on the orientation of the molecule. These properties are common in the free electron model and the model with Coulomb interactions. (3) The spectrum of C70 averaged over bond disorder and random orientations is compared with experiments in a solution. There is an overall agreement about the spectral shape. Differences in the spectra of C60 and C70 are discussed in connection with the symmetry reduction from a soccerball to a rugbyball.