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DOE OSTI · 3022560

Dynamic Atomistic Polar Structure Underpins Ultrahigh Linear Electro-Optic Coefficient in Transparent Ferroelectric Ceramics

Abstract

Transparent ferroelectrics with high linear electro-optic (EO) coefficients are critical for advanced electro-optical devices. However, achieving optical transparency in ferroelectric ceramics remains challenging due to visible light scattering caused by defects such as domain walls, grain boundaries, and pores. Here, we report the successful fabrication of transparent ferroelectric ceramics through innovative chemical composition design and an advanced two-step sintering process in the La-doped Pb(Mg 1/3 Nb 2/3 )O 3 –PbTiO 3 system. The optical transparency, which is near the theoretical upper limit, can be attributed to the wide band gap and the minimization of light scattering of defects. By minimizing porosity and engineering grain/domain sizes to differ significantly from the wavelengths of visible light, we suppress scattering, achieving optical transparency near the theoretical upper limit. Strikingly, these ceramics exhibit an ultrahigh linear EO coefficient of ∼1417 pm/V, over 65 times greater than that of LiNbO 3 single crystals, the current industry standard. We attribute this exceptional performance to dynamic atomistic polar structures within switchable, thermally stable domains, which enhance electronic polarization sensitivity. This mechanism is corroborated by dielectric spectroscopy, high-resolution transmission electron microscopy and simulation. Our findings offer insights into the design of cost-effective transparent materials with exceptional EO properties, paving the way for next-generation electro-optical devices.

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BibTeXRIS

Jiang, Qinghui [Huazhong University of Science and Technology, Wuhan (China)] (ORCID:0000000178512653), Zhao, Weigang [Xi’an Jiaotong University (China)], Zhang, Man [Queen Mary University of London (United Kingdom)], Zhou, Jian-Ping [Shaanxi Normal University, Xi’an (China)] (ORCID:0000000308071404), Liao, Mingqing [Jiangsu University of Science and Technology, Zhenjiang (China)] (ORCID:0000000197653400), Smolyanyuk, Andriy [TU Wien, Vienna (Austria)], Wu, Zixuan [Queen Mary University of London (United Kingdom)] (ORCID:0009000958295642), Jia, Chenglong [Lanzhou University (China)] (ORCID:000000032064923X), Wei, Xiaoyong [Xi’an Jiaotong University (China)], Weber, Cedric [The Australian National University (Australia)] (ORCID:0000000269892700), Tarakina, Nadezda V. [Max Planck Institute of Colloids and Interfaces, Potsdam (Germany)] (ORCID:000000022365861X), Abrahams, Isaac [Queen Mary University of London (United Kingdom)] (ORCID:0000000286066056), Tomczak, Jan M. [King’s College London (United Kingdom); TU Wien, Vienna (Austria)], Liu, Zi-Kui [The Pennsylvania State University, University Park, PA (United States)], Roddatis, Vladimir [GFZ Helmholtz Centre for Geosciences, Potsdam (Germany)] (ORCID:0000000295840808), Yan, Haixue [Queen Mary University of London (United Kingdom)] (ORCID:0000000245631100). 2025-11-04. Dynamic Atomistic Polar Structure Underpins Ultrahigh Linear Electro-Optic Coefficient in Transparent Ferroelectric Ceramics. https://doi.org/10.1021/jacs.5c15699

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36 MATERIALS SCIENCE↗