Abstract: A combinatorial synthesis system is provided which combines pulsed laser deposition techniques with the continuous composition spread technique in which a plurality of targets made of different ingredient materials are arranged in a predetermined relationship and are ablated by an energetic beam focused on the surface of a particular target. By maintaining the energetic beam in a stationary state, the target carousel is rotated so as to bring a particular target in engagement with the energetic beam. The targets are brought into engagement with the energetic beam in a predetermined sequence so that different materials are deposited onto the substrate in a predetermined sequence. Distributed deposition areas surround each deposition center and overlap each with the other to form a continuous compositional spread on the surface of the substrate.