The present study reports the development of a laser assisted ultrasonic spray pyrolysis technique and synthesis of dense optical alumina films using the same. In this technique ultrasonically generated aerosols of aluminum acetylacetonate dissolved in ethanol and a laser beam (Nd: YAG, CW, 1064 nm) were fed coaxially and concurrently through a quartz tube on to a hot substrate mounted on an X-Y raster stage. At the laser focused spot the precursor underwent solvent evaporation and solute sublimation followed by precursor vapor decomposition giving rise to oxide coating, the substrate is rastered to get large surface area coating. The surface morphology revealed coalescence of particles with increase in laser power. The observed particle sizes were 17 nm for films synthesized without laser and 18, 21 and 25 nm for films made with laser at 25, 38 and 50 W, respectively. Refractive index of the films synthesized increased from 1.56 to 1.62 as the laser power increased from 0 to 50 W. The stoichiometry of films was studied using XPS and the increase in interfacial layer thickness with laser power was observed from dynamic SIMS depth profiling and ellipsometry. (C) 2012 Elsevier B.V. All rights reserved.