A thorough investigation of polysilicon films crystallized from amorphous silicon using a XeCl excimer laser has been completed. Emphasis was placed on the development of large crystals, good uniformity, and low surface roughness, with an eye towards improving throughput. This was accomplished through use of SiO2 barrier layers, multiple passes, and careful consideration of annealing ambient. Thermal modeling was performed to help interpret the observed trends and aid in optimization. By controlling these process parameters, samples were produced with a high degree of uniformity and two-dimensional structural ordering, with grains nearly identical in size and stacked in rows and columns. However, a biproduct of the ordering was the creation of large topographical features at the intersection points of multiple grain boundaries, which lead to surface roughness in the range of 12 nm. By applying more shots to the same area, films with maximum grain sizes on the order of 3 μm and reduced surface roughness (6 nm) were realized. © 1997 American Institute of Physics.