Using reactive pulsed laser deposition assisted by electron cyclotron resonance (ECR) plasma, we have synthesized GaN thin films from a polycrystalline GaAs target at low temperatures. This was achieved by ablating the GaAs target in the reactive environment of a nitrogen plasma generated from ECR microwave discharge in pure nitrogen gas and depositing the films with concurrent bombardment by the low-energy nitrogen plasma stream. High-energy ion backscattering spectroscopy analysis shows that the synthesized films are gallium rich. Characterizations by x-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy confirm the presence of GaN bonds in the films. The recorded absorption spectrum also reveals GaN stretching mode characteristic of the hexagonal GaN phase. The synthesized GaN films are transparent in the visible region and have a band gap of 3.38 eV. Optical emission from the plume during film deposition reveals that the plume created by pulsed laser ablation of the GaAs target consists mainly of monoatomic atoms and ions of gallium and arsenic. Mechanisms responsible for the formation of GaN molecules and the growth of GaN films are also discussed. (c) 2005 American Vacuum Society.