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[Display omitted] • Atomic scale smoothing of GaN is realized by plasma-based atom-selective etching. • Temperature is a key factor in determining the PASE etching mode of GaN. • Sa roughness can be reduced from 135.8 nm to 0.527 nm by 2 min of PASE. • PASE demonstrates an extremely high MRR of 93.01 μm/min. Plasma-based atom-selective etching (PASE) of GaN is conducted to realize the highly efficient planarization of the GaN surface. Inductively coupled plasma with high temperature and high concentration of radicals is used as the source of PASE. The non-toxic carbon tetrafluoride is chosen over chlorine as the reaction gas, and the volatility of the etching products will be improved at high temperatures in the PASE of GaN. After 2 min of PASE, the GaN surface roughness is reduced from Sa 135.8 nm to Sa 0.527 nm. The material removal rate of PASE of GaN is measured to be 93.01 μm/min, thousands of times higher than that of the conventional chemical mechanical polishing method. The crystal structure of the GaN subsurface is well-ordered without any damage or defects. PASE is thus proven to be a non-destructive etching method. In this study, the effects of radio frequency power and reaction gas flow rate on PASE are also investigated. Surface temperature and concentration of radicals are found to be the critical factors in the PASE of GaN. [ABSTRACT FROM AUTHOR]