Studies of fullerene absorption and production using an infrared free-electron laser

Tunable photon sources such as free-electron lasers are potentially valuable tools in spectroscopic studies of fullerenes, a new class of carbon materials with unique cage structures. We have used the infrared free-electron-laser facility at Vanderbilt University to study the infrared absorption of gas-phase fullerene molecules and also to investigate the effects of an infrared laser in the synthesis and crystallization of fullerene materials. In one experiment, fullerene vapor was created in a heat pipe through which the FEL beam was passed; the transmission of the FEL beam relative to a reference detector was measured as a function of wavelength. A large (>10%) absorption of the IR laser was observed when it passed through C60 vapor at ∼800 degrees C. Due to the broad spectral width of the FEL as well as spectral congestion, no spectral peaks were seen when the laser wavelength was tuned across a T1uC60 IR mode near 7.0 μ. However, it is expected that the vibrational features can be resolved experimentally by passing the transmitted beam through a monochromator. In a separate experiment, the FEL beam was focused onto a surface of graphite or graphite/metal mixture target. Various fullerene molecules, including endohedral types, were produced when the soot was recovered from the ablation chamber. The yield of the products was measured to be ∼0.4 g/J of the incident laser energy. However, both the yield and the product distribution are virtually, the same as those in experiments using a nanosecond Nd:YAG laser. This suggests that the laser wavelength is not a crucial parameter in making fullerenes by laser ablation. Even when the laser is at resonance with one of the vibrational modes of C60, the fullerene production is neither substantially enhanced nor suppressed