The shear-thickening polishing (STP) method, a flexible polishing technique developed in recent years, was utilized to obtain high surface quality of yttrium aluminum garnet (YAG) crystal effectively. The effect of polishing slurry pH value, which characterizes the chemical action between slurry and YAG crystal, on the material removal rate and surface roughness of YAG crystal was investigated, and the mechanism of the chemical action between YAG and slurry in STP process was revealed through X-ray photoelectron spectroscopy (XPS) analysis. The influence of polishing speed and abrasive concentration, which were relating with mechanical action, on the polishing effects was also studied. The experimental results show that when the pH value of the polishing slurry is lower than 11, the dissociation of chemical bonds and the formation of new bonds on the surface of the YAG crystal are predominantly found, resulting in a lower material removal rate. While the pH value of polishing slurry reaches 13, a reaction layer consisting of Al2SiO5 and Y2SiO5, which has lower hardness than abrasive, is formed on the surface, and this reaction layer can be removed by mechanical action efficiently. The surface roughness Sa decreases from 60 ± 10 nm to 0.38 ± 0.06 nm in 15 min with MRR reaches 117.30 nm/min, which is 4.3 times higher than that of chemical mechanical polishing. Based on the results of XPS analysis, the material removal mechanism of YAG polished by STP is proposed. As revealed by the results, STP with chemical action provide a high efficiency polishing method for the high surface quality YAG crystal.
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