Effect of rare-earth doping on the structural and optical properties of the Ag3AsS3 crystals

Non-linear optical (NLO) materials allow the production of the coherent laser beam in the difficult frequency ranges of the electromagnetic spectrum. Aiming to explore new classes of the NLO materials with high optical performance in the infrared region, in this work, we investigated the effect of the rare earth doping (Pr, Eu, Yb) on the crystal structure and optical properties of the Ag3AsS3 crystals. The performed analysis of the XRD patterns indicates that the rare earth elements are located in the Ag sites of the crystal lattice. As a result, the second harmonic generation intensity, which determines the effectiveness of the NLO materials, increases with the increase of rare earth dopant content up to 1.0%. Using the absorption analysis and Raman spectroscopy, we show that the increase in the SHG intensity can be related to the slight decrease of the bandgap, as well as with the increased electron-phonon interaction in rare-earth-doped Ag3AsS3 crystals. Considering the discovered enhancement of the SHG intensity, accompanied by the low melting temperature, this work offers rare-earth-doped Ag3AsS3 crystals as potential candidates for the non-linear optical applications for the infrared frequency range.