We have studied theoretical photoelectron-momentum distributions of C-60 using time-dependent density functional theory (TDDFT) in real time and including a self-interaction correction. Our calculations furthermore account for a proper orientation averaging allowing a direct comparison with experimental results. To illustrate the capabilities of this direct (microscopic and time-dependent) approach, two very different photo-excitation conditions are considered: excitation with a high-frequency XUV light at 20 eV and with a low-frequency IR femtosecond pulse at 1.55 eV. The interaction with the XUV light leads to one-photon transitions and a linear ionization regime. In that situation, the spectrum of occupied single-electron states in C-60 is directly mapped to the photoelectron spectrum. On the contrary, the IR pulse leads to multiphoton ionization in which only the two least-bound states contribute to the process. In both dynamical regimes (mono- and multiphoton), calculated and experimental angle-resolved photoelectron spectra compare reasonably well. The observed discrepancies can be understood by the theoretical underestimation of higher-order many-body interaction processes such as electron-electron scattering and by the fact that experiments are performed at finite temperature. These results pave the way to a multiscale description of the C-60 ionization mechanisms that is required to render justice to the variety of processes observed experimentally for fullerene molecules.
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