An electro-optic (EO) modulator is one of the most important optical devices and has been widely used in the photonic industry. Performance of EO modulators mainly depends on the property of EO materials. Here, the EO property of the (111)-oriented single domain rhombohedra phase (1-x)Pb(Mg1/3Nb2/3)O3-xPbTiO3 (PMN-PT) single crystal is investigated. Due to the light scattering by domain walls, a single domain crystal is essential and has been well prepared here by a thermal annealing and high temperature poling process. It is found that domains become irregular with significantly decreased dimension after annealing, which indicates that the ferroelastic domain walls are eliminated. A crack-free single domain crystal shows excellent optical quality, with a high transmittance of approximately 70% in near-infrared regions. Finally, the effective EO coefficient of the (111)-oriented rhombohedral phase PMN-PT crystal is measured by a Senarmont compensator amplitude modulator. An effective EO coefficient of 112 pm/V is obtained in the (111)-oriented rhombohedral phase PMN-PT crystal, which is much higher than that of the commercial LiNbO3 crystal, indicating the potential for use in compact and low driving voltage EO devices.

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