Contrasting behavior of covalent and molecular carbon allotropes exposed to extreme ultraviolet and soft x-ray free-electron laser radiation

Abstract

All carbon materials, e.g., amorphous carbon (a-C) coatings and ${\mathrm{C}}_{60}$ fullerene thin films, play an important role in short-wavelength free-electron laser (FEL) research motivated by FEL optics development and prospective nanotechnology applications. Responses of a-C and ${\mathrm{C}}_{60}$ layers to the extreme ultraviolet (SPring-8 Compact SASE Source in Japan) and soft x-ray (free-electron laser in Hamburg) free-electron laser radiation are investigated by Raman spectroscopy, differential interference contrast, and atomic force microscopy. A remarkable difference in the behavior of covalent (a-C) and molecular (${\mathrm{C}}_{60}$) carbonaceous solids is demonstrated under these irradiation conditions. Low thresholds for ablation of a fullerene crystal (estimated to be around 0.15 eV/atom for ${\mathrm{C}}_{60}$ vs 0.9 eV/atom for a-C in terms of the absorbed dose) are caused by a low cohesive energy of fullerene crystals. An efficient mechanism of the removal of intact ${\mathrm{C}}_{60}$ molecules from the irradiated crystal due to Coulomb repulsion of fullerene-cage cation radicals formed by the ionizing radiation is revealed by a detailed modeling.