Imaging of fullerenes

High-harmonic generation is studied as a tool to image molecular structure on an ultrafast time scale. Harmonic signals generated in highly symmetric fullerenes (C20 to C180) using an extension of the so-called Lewenstein model exhibit modulations in the plateaus of the spectra at mid-infrared wavelengths (upper panel). Theoretical analysis of the results has shown that the minima are due to multislit interference effects arising from the contributions of the different atomic centers to the dipole moment. The modulations disappear if the atomic contributions are added incoherently (middle panel). The position of the minima are found to be in good agreement with those in the recombination matrix element (lower panel), which can be used to retrieve the radius of the fullerenes from the spectra.

M.F. Ciappina et al., Phys. Rev. A 76 (2007) 063406; ibid. 78 (2008) 063405