A new cluster time-of-flight secondary ion mass spectrometry (TOF-SIMS) was developed using a size-selected gas cluster ion as a projectile. Since a large gas cluster ion can generate many low-energy constituent atoms in a collision with the surface, it causes multiple and ultra low-energy sputtering. The mean kinetic energy of constituent atoms is provided by dividing the acceleration energy of the gas cluster ion by the number of constituent atoms. Therefore, the sputtering can be controlled to minimize the decomposition of sample molecules and substrate material by precisely adjusting the number of constituent atoms (the cluster size) and/or acceleration energy of the gas cluster ion. The cluster size was selected on the basis of the time-of-flight method using two ion deflectors attached along the ion-beam line. A high resolution of 11.7 was achieved for the cluster size/size width (M/Delta M) of Ar-cluster ions. (C) 2008 Elsevier B. V. All rights reserved.