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This paper outlines notable advances in the wire electrical discharge machining of polycrystalline silicon workpieces for wafer preparation. Our use of assisting electrodes permits the transfer of aluminum particles to the machined surface of the polycrystalline silicon workpieces, to enhance conductivity and alter surface topography regardless of the silicon’s crystallographic structure and diamond-type lattice. This in-process surface modification technique was shown to promote material removal and simultaneously preserve the integrity of the machined surfaces with preferable surface textures. In the validation experiment, the 25 mm-thick assisting electrodes deposited a notable concentration of aluminium on the machined surface (~3.87 wt %), which greatly accelerated the rate of material removal (~9.42 mg/s) with minimal surface roughness (Sa ~5.49 μm) and moderate skewness (−0.23). The parameter combination used to obtain the optimal surface roughness (Sa 2.54 μm) was as follows: open voltage (80 V), electrical resistance (1.7 Ω), pulse-on time (30 μs), and electrode thickness (15 mm). In multiple objective optimization, the preferred parameter combination (open voltage = 80 V, resistance = 1.4 Ω, pulse-on time = 60 μs, and assisting electrode thickness = 25 mm) achieved the following appreciable results: surface modification of 3.26 ± 0.61 wt %, material removal rate of 7.08 ± 2.2 mg/min, and surface roughness of Sa = 4.3 ± 1.67 μm.

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