The temperature characteristics of dielectric constants, spontaneous polarization, thermal‐expansion coefficients, indices of refraction, and optical rotatory power of Pb5Ge3O11 single crystals have been investigated in detail from room temperature up to above the Curie temperature, 177°C. From the results of these measurements, the following constants were obtained: linear thermal‐expansion coefficients (αa)F=7.75×10−6/deg°C and (αc)F=7.79×10−6/deg°C (ferroelectric phase), (αa)P=13.8×10−6/deg°C and (αc)P=13.4×10−6/deg°C (paraelectric phase); quadratic electro‐optic constants g33T=0.47×108cm4 /C2, g13T=0.37×108cm4 /C2; and electrogyration coefficient γ33 =8.7 cm2/C. An isomorphous compound Pb5(Ge2O7)(SiO4) was synthesized and was found to be ferroelectric with Tc=60°C and Ps=1.7 μC/cm2 at room temperature. Ferroelectric properties and electrogyration coefficient were studied in the solid‐solution system Pb5(Ge2O7)(GeO4)1−x (SiO4)x.

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