Chalcogenide Glasses Based on Germanium Disulfide for Second Harmonic Generation

High second‐order susceptibilities are created by thermal poling in bulk germanium disulfide based chalcogenide glasses. Experimental conditions of the poling treatment (temperature, voltage, time) were optimized for each glass composition. The second‐order nonlinear signals were recorded by using the Maker fringes experiment and a second‐order coefficient χ⁽²⁾ up to 8 pm V^–1 was measured in the Ge₂₅Sb₁₀S₆₅ glass. This value is obtained using a simulation based on accurate knowledge of the thickness of the nonlinear layer. Two mechanisms are proposed to explain the creation of a nonlinear layer under the anode: the formation and the migration of charged defects towards the anode may mainly occur in Ge₂₀Ga₅Sb₁₀S₆₅ and Ge₂₅Ga₅S₇₀ glasses, whereas the migration of Na⁺ ions towards the cathode may be responsible for the accumulation of negative charges under the anode in Ge₃₃S₆₇ and Ge₂₅Sb₁₀S₆₅ glasses. Different electronic conductivity behaviors seem to be at the origin of the phenomenon. In parallel, the potential effect of the poling treatment on the structural and electronic properties is studied using Raman spectroscopy and secondary ion mass spectroscopy measurements.