First-principles quantum molecular-dynamics study of the vibrations of icosahedralC60

Abstract

Using first-principles real-space quantum-molecular-dynamics, we compute the structure and normal modes of icosahedral ${\mathrm{C}}_{60}$. The many-electron ground-state energy and atomic forces are computed for each atomic configuration, and the results are used in molecular-dynamics calculations of the modes. We focus here on the 14 modes which are either first-order Raman active or infrared active, and we compare our calculated mode frequencies with experimental data. Using no free parameters, we compute the frequencies to between 4% and 16% of their measured values, depending on the mode.