DOE OSTI · 3012961
Colossal Cryogenic Electro‐Optic Response Through Metastability in Strained BaTiO 3 Thin Films
Abstract
The search for thin film electro-optic materials that can retain superior performance under cryogenic conditions has become critical for quantum computing. Barium titanate thin films show large linear electro-optic coefficients in the tetragonal phase at room temperature, which is severely degraded down to ≈200 pm V −1 in the rhombohedral phase at cryogenic temperatures. There is immense interest in manipulating these phase transformations and retaining superior electro-optic properties down to liquid helium temperature. Utilizing the thermodynamic theory of optical properties, a large low-temperature electro-optic response is designed by engineering the energetic competition between different ferroelectric phases, leading to a low-symmetry monoclinic phase with a massive electro-optic response. The existence of this phase is demonstrated in a strain-tuned BaTiO 3 thin film that exhibits a linear electro-optic coefficient of 2516 ± 100 pm V −1 at 5 K, which is an order of magnitude higher than the best reported performance thus far. Importantly, the electro-optic coefficient increases by 100 × during cooling, unlike the conventional films, where it degrades. Further, at the lowest temperature, significant higher order electro-optic responses also emerge. These results represent a new framework for designing materials with property enhancements by stabilizing highly tunable metastable phases with strain.
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Suceava, Albert [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000176619596), Hazra, Sankalpa [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000291268058), Ross, Aiden [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0009000181956172), Philippi, Ian Reed [Pennsylvania State University University Park PA 16802 USA], Sotir, Dylan [Cornell Univ., Ithaca, NY (United States)] (ORCID:0000000175758885), Brower, Brynn [Pennsylvania State Univ., University Park, PA (United States)], Ding, Lei [Pennsylvania State Univ., University Park, PA (United States)], Zhu, Yingxin [Pennsylvania State Univ., University Park, PA (United States)], Zhang, Zhiyu [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:000900018537417X), Sarkar, Himirkanti [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000340847532), Sarker, Saugata [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000168121747), Yang, Yang [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000200255914), Sarker, Suchismita [Cornell Univ., Ithaca, NY (United States)] (ORCID:0000000288201143), Stoica, Vladimir A. [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000227347819), Schlom, Darrell G. [Cornell Univ., Ithaca, NY (United States); Leibniz Inst. for Crystal Growth (IKZ), Berlin (Germany)] (ORCID:0000000324936113), Chen, Long‐Qing [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000333593781), Gopalan, Venkatraman [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000168663677). 2025-10-11. Colossal Cryogenic Electro‐Optic Response Through Metastability in Strained BaTiO 3 Thin Films. https://doi.org/10.1002/adma.202507564
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