The electro-optic (E-O) response is fundamental where the refractive index of materials can be modulated by the external electric field. Up to now, E-O modulation has become a critical technology in photonics, quantum optics, modern communication, etc. However, the design of E-O crystals with broadband availabilities and large E-O effect is still challenging since the E-O response is contributed by both electrons and phonons. Here, an electron-lattice synergistic coordination strategy is proposed for boosting the E-O response, and with the langasite as the subject, a novel crystal La3Zr0.5Ga5Si0.5O14 (LZGS) is designed. By the rational introduction of the Zr4+ ion in the octahedral site, it is found that the E-O response can be obviously improved attributed to the active 4d orbitals of the Zr4+ ion and the optical phonons of the flexible (ZrO6) unit. This crystal also has advantages in transparency, laser damage threshold and E-O coefficient compared with the well-known E-O crystals. Moreover, broadband E-O modulation is also demonstrated in the lasers at wavelengths from 639 to 1991nm. These findings not only demonstrate an excellent E-O crystal for the development of modern devices in classical and quantum fields but also provide a design strategy for boosting the E-O response.
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