The properties of femosecond-pulsed laser deposited GaAs nanoclusters were investigated. Nanoclusters of GaAs were produced by laser ablating a single crystal GaAs target in vacuum or in a buffer gas using a Ti-sapphire laser with a 150 fs minimum pulse length. For in-vacuum deposition, X-ray diffraction (XRD), scanning electron microscopy (SEM), and atomic force microscopy (AFM) revealed that the average cluster size was approximately 7 nm for laser pulse lengths between 150 A and 25 ps. The average cluster size dropped to approximately 1.5 nm at a pulse length of 500 ps. It was also observed that film thickness decreased with increasing laser pulse length. A reflective coating, which accumulated on the laser admission window during ablation, reduced the amount of laser energy reaching the target for subsequent laser shots and developed more rapidly at longer pulse lengths. This observation indicates that non-stoichiometric (metallic) ablatants were produced more readily at longer pulse lengths. The angular distribution of ejected material about the target normal was well fitted to a bi-cosine distribution of cos(47) theta + cos(4) theta for ablation in vacuum using 150 fs pulses. XPS and AES revealed that the vacuum-deposited films contained excess amorphous Ga or As in addition to the stoichiometric GaAs nanocrystals seen with XRD. However, films containing only the GaAs nanocrystals were produced when ablation was carried out in the presence of a buffer gas with a pressure in excess of 6.67 Pa. At buffer gas pressure on the order of I Torr, it was found that the stoichiometry of the ablated target was also preserved. These experiments indicate that both laser pulse length and buffer gas pressure play important roles in the formation of multi-element nanocrystals by laser ablation. The effects of gas pressure on the target's morphology and the size of the GaAs nanocrystals formed will also be discussed. (C) 2003 Elsevier B.V. All rights reserved.