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Centimeter-sized Er-doped single crystals were grown from the melts GaSe:Er(0.025, 0.1, 0.5, 1 and 2at%) by modified vertical Bridgman technology. Real Er content is ascertained as 0.009, 0.019, 0.033, 0.042 and 0.048at%, respectively. Solubility of Er in GaSe does not exceed 5×10−4. Optimal doping of 0.033at% of Er was established from SHG experiment. Improved optical quality is identified as a reason of increased nonlinearity for about 24% to that in pure GaSe. New Raman scattering band is found at 2900cm−1 that properly related to 4F9/2→4I9/2 transition of Er3+ ion.