High-order harmonic generation (HHG) has unleashed the power of strong laser physics in solids. Here we investigate HHG from a large system, solid ${\mathrm{C}}_{60}$, with 240 valence electrons engaging harmonic generation at each crystal momentum. We employ the density functional theory and the time-dependent Liouville equation of the density matrix to compute HHG signals. We find that under a moderately strong laser pulse, HHG signals reach 15th order, consistent with the experimental results from ${\mathrm{C}}_{60}$ plasma. The helicity dependence in solid ${\mathrm{C}}_{60}$ is weak, due to the high symmetry. In contrast to the general belief, HHG is unsuitable for band structure mapping in ${\mathrm{C}}_{60}$. However, we find a window of opportunity using a long wavelength, where harmonics are generated through multiple-photon excitation. In particular, the fifth-order harmonic energies closely follow the transition energy dispersion between the valence and conduction bands. This finding is expected to motivate future experimental investigations.

• Received 6 January 2020
• Accepted 14 February 2020

DOI:https://doi.org/10.1103/PhysRevB.101.081412