Azo-dye compounds, in bulk or as thin films, are extensively studied due to their particular optical properties. These properties include non-linear interaction, e.g. two-photon absorption, optical limiting and all-optical poling, with potential applications in optoelectronics and sensors development. Herein, we report on the deposition of pyrazolone derivatives, namely 1-phenyl-3-methyl-4-(1'-azo-2'-sodium carboxylate)-pyrazole-5-one thin films, for applications in second harmonic generation. Matrix-assisted pulsed laser evaporation was employed for layers growth, using a Nd:YAG device operating at 266 nm (4 omega). The structure and surface morphology of the deposited films were examined by Fourier transform infrared spectroscopy, atomic force microscopy, and scanning electron microscopy. Spectroscopic-ellipsometry was employed to investigate thin film optical properties. Significant second harmonic generation capabilities of the compound were pointed out by using a femtosecond Ti:sapphire laser. (C) 2013 Elsevier B.V. All rights reserved.