Cooperative roles of chemical reactions and mechanical friction in chemical mechanical polishing of gallium nitride assisted by OH radicals: tight-binding quantum chemical molecular dynamics simulations

Chemical mechanical polishing (CMP) is a key manufacturing process for applying gallium nitride (GaN), especially the Ga-face GaN, to semiconductor devices such as laser diodes. However, the CMP efficiency for GaN is very low due to its high hardness and chemical stability. Experimentally, OH radicals appear able to improve the CMP efficiency of GaN polished by a SiO₂abrasive grain, whereas the mechanisms of the OH-radical-assisted CMP process remain unclear because experimental elucidation of the complex chemical reactions occurring among GaN substrate, abrasive grain, and OH radicals is difficult. In this work, we used our previously developed tight-binding quantum chemical molecular dynamics simulator to study the OH-radical-assisted CMP process of the widely employed Ga-face GaN substrate polished by an amorphous SiO₂abrasive grain in an effort to understand how OH radicals assist the CMP process and then aid the development of next-generation CMP techniques. Our simulations revealed that the OH-radical-assisted CMP process of GaN occursviathe following three basic reaction steps: (i) first, all hydrogen terminations on the GaN surface are replaced by OH terminations through continuous reactions with OH radicals; (ii) after the substrate is fully terminated by OH, the hydrogen atoms of these OH terminations are removed by reacting with newly added OH radicals, which forms H₂O molecules and leaves energetic oxygen atoms with dangling bonds on the surface; and (iii) finally, these energetic oxygen atoms intrude inside the substrate with concomitant dissociation of Ga-N bonds and the generation of N₂and gallium hydroxide molecules, which accumulatively lead to the removal of N and Ga atoms from the substrate.