The
effect of native defect density on structure evolution during
oxidation has not been systematically studied for two-dimensional
(2D) materials. Photo-oxidation provides a way to fasten oxidation
in 2D materials. The oxidation dynamics in atomically layered GaSe
is systemically studied here through the temporal evolution of Raman
spectroscopy. Two stages of oxidation processes are observed under
above-gap laser irradiation in ambient conditions. First, the Raman
intensity in GaSe flakes linearly decreases with the square root of
oxidation time, and the slope shows a linear dependence on the square
root of laser power. This stage is associated with photo-oxidation-induced
structural damage with the formation of randomly distributed oxidation
products, i.e., Ga2Se3, Ga2O3, and crystalline and amorphous selenium. A model is proposed
to interpret the oxidation kinetics in GaSe flakes in terms of illumination
time, laser power, and native defect density. Second, continuous change
in slope is observed, which is due to the oxidative products merging
to form a large oxidation lump. The evolution of defect density in
GaSe flakes in terms of laser power, oxidation time, and native defect
density during oxidation shines new light on the understanding of
the stabilities of 2D materials in ambient environments.