A large variety of ultrafast laser‐matter interaction regimes and different processed surface finishing qualities of stainless steel can be achieved by varying the laser processing parameters. The optimization of the laser fluence to the most efficient ablation also leads to the lowest surface roughness of the ablated material. High laser fluence together with a high pulse repetition rate leads to heat accumulation, which results in the formation of microstructures with various morphology and scales. The use of GHz bursts allows a rough stainless‐steel surface to be smoothed and even polished. In this work, the fast and high‐quality milling of 2.5D cavities is demonstrated. Laser beam spot optimization is used to increase the throughput of the high‐power femtosecond laser (67.8 W), resulting in an ablation rate of 13 mm3 min−1. The complex cavities are produced by laser milling and cutting in layers. The formation of surface structures on stainless steel because of laser irradiation has been demonstrated. The possibilities of further GHz burst polishing are examined on previously laser‐milled stainless steel using with lowest possible surface roughness. The ability to polish the surface with microstructures below the original roughness is demonstrated by bursts of ultrashort pulses with a repetition rate in the GHz range. It has been demonstrated that mold milling in stainless steel designed for LED diffusers can be fabricated using a modern femtosecond laser source together with beam size optimization technique for efficient ablation with low surface roughness, layer‐by‐layer milling techniques, and GHz burst polishing techniques.
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