Strong electro-optical (EO) anisotropy has been measured in (1−x)Pb(Mg1/3Nb2/3)O3–xPbTiO3 [(1−x)PMN–xPT] single crystalline films epitaxially grown on (100)-cut LaAlO3 substrate, through using an improved dynamic alternating-current ellipsometric null EO detection technique with high accuracy. Large quadratic EO coefficients, which can be as large as 1.38×10−16 (m/V)2 in 0.67PMN–0.33PT film, were obtained in all the used compositions when electric field was applied along {110} directions. The strong EO anisotropy has been explained according to the structural relationship between ferroelectric polarization, input light polarization, and the applied electric field.
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