The interaction of the highly energetic pulsed excimer laser beam with a target material induces non-equilibrium physico-chemical processes which could be harnessed to synthesize a variety of novel and technologically attractive materials that are difficult to grow using more conventional thin film deposition techniques. In this paper, recent advances on two excimer laser based techniques that we have used in the processing of thin films and surfaces will be presented. First, we demonstrate the synthesis, by Pulsed Laser Melting (PLM), of silicon supersaturated with sulfur at concentrations several orders of magnitude greater than the solubility limit of silicon alloys, with strong sub-bandgap optical absorption. This material has potential applications in the fabrication of Si-based opto-electronic devices. Second, the capability of Remote Plasma Pulsed Laser Deposition (RP-PLD) in synthesizing the meta-stable half-metallic CrO2 compound that is of great interest in the field of spintronics was assessed. Infra-Red spectroscopy and Magnetic Force Microscopy indicate that the use of the remote plasma is beneficial to the formation of the CrO2 phase, at a deposition pressure of 30 mTorr and for deposition temperature below 350 °C. Atomic Force Microscopy and Magnetic Force Microscopy studies respectively show that films containing the CrO2 phase have significantly different surface topography and magnetic characteristics from those in which the Cr2O3 phase is dominant.© (2007) COPYRIGHT SPIE--The International Society for Optical Engineering. Downloading of the abstract is permitted for personal use only.