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A combination of experimental and computational methods was performed to investigate the defect and optical properties of S-doped and Al-doped GaSe crystals. Our experimental and calculated results indicate that the doped S and Al atoms can form SSe and AlGa+ substitutional defects in the layered GaSe structure. The non-isovalent AlGa+ defect can strengthen the chemical bonding within the intralayer and induce complex defects within the interlayer in the layered GaSe structure. Al-doping maximally improves the hardness of GaSe, which makes it a promising nonlinear frequency conversion material in the infrared and THz ranges. The isovalent SSe defect determines the GaSe1−xSx mixed structure. Calculated results indicate that the refractive index of GaSe1−xSx decreases with the x value, while the band gap increases. The unique properties of GaSe1−xSx may make it a potential candidate for double heterojunction photoelectric materials.

Experimental and theoretical investigations on the defect and optical properties of S- and Al-doped GaSe crystals