We analyzed TOF-SIMS spectra obtained from three different size of fullerenes (C-60, C-70 and C-84) by using Ga+, Au+ and Au-3(+) primary ion beams and investigated the fragmentation patterns, the enhancement of secondary ion yields and the restraint of fragmentation by using cluster primary ion beams compared with monoatomic primary ion beams. In the TOS-SIMS spectra from C-70 and C-84, it was found that a fragment ion, identified as C-60(+) (m/z = 720), showed a relatively high intensity compared with that of other fragment ions related to C-2 depletion. It was also found that the Au-3(+) bombardment caused intensity enhancement of intact molecules (C-60(+), C-70(+) and C-84(+)) and restrained the fragmentation due to C-2 depletion. (C) 2008 Elsevier B. V. All rights reserved.