This study demonstrates an innovative approach to clean a polycrystalline seed layer surface for solid phase epitaxy of amorphous silicon (a-Si). The excimer laser cleaning (ELC) makes use of in situ excimer laser irradiation during the first stages of a-Si deposition leading to melting of the as deposited a-Si and parts of the seed layer. The increased diffusion in liquid silicon allows for “smearing out” of surface contamination species. After liquid phase epitaxy is finished, further a-Si is deposited and crystallized by solid phase epitaxy. Thanks to the “smearing out,” the interface between the crystalline and amorphous silicon exhibits less contamination locally. SIMS measurements demonstrate a reduced carbon concentration at the seed layer surface after ELC. Numerical simulations, taking into account heat transfer and temperature dependent diffusion, support the reduction of carbon concentration. The simulations agree very well with experimental results. To get optimal solid phase growth conditions, the a-Si deposition temperature has to be below 200 °C. Above 200 °C deposition temperature, defective growth occurs resulting in poor crystallinity or even in nonepitaxial growth.