Orientation dependence of energy absorption and relaxation dynamics of C₆₀ in fs-laser pulses: How round is C₆₀?

By means of non-adiabatic quantum molecular dynamics it is shown, that the amount of energy deposited into $\text{C}_{60}$ by a short laser field strongly depends on the molecular orientation with respect to the laser polarization direction. In consequence, subsequent electron-vibration coupling leads to different nuclear relaxation mechanisms with mainly three pathways: (1) excitation of giant $\text{A}_g(1)$ modes ("breathing"), (2) formation of deformed cage-like complexes ("isomers"), fragmentation predominantly into two large pieces ("fission"). The results are in accord with and explain nicely already existing experimental data. Future experiments are proposed to confirm the detailed predictions.